1-s2.0-s0926860x13004432-main (1)

Upload: ysabel-huaccallo-aguilar

Post on 14-Apr-2018

216 views

Category:

Documents


0 download

TRANSCRIPT

  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    1/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    Applied Catalysis A: General xxx (2013) xxxxxx

    Contents lists available at ScienceDirect

    Applied Catalysis A: General

    j ournal homepage : www.elsevier .com/ locate /apcata

    Critical evaluation ofthe role ofthe distribution ofAl atoms in theframework for the activity ofmetallo-zeolites in redox N2O/NOxreactions

    Zdenek Sobalik, Petr Sazama,Jiri Dedecek, BlankaWichterlov

    J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, CZ-182 23 Prague 8, Czech Republic

    a r t i c l e i n f o

    Article history:Received 28 February 2013

    Received in revised form 6 June 2013

    Accepted 16 July 2013

    Available online xxx

    Keywords:

    Cu-zeolite

    Co-zeolite

    Fe-zeolite

    SCR-NOx

    NO decomposition

    N2O decomposition

    Al distribution in theframework

    Al pairs in zeolites

    ZSM-5

    Thebeta zeolite

    a b s t r a c t

    Both the laboratory synthesized zeoliteswith tailoreddistributionofframeworkAlatoms andcommercial

    ZSM-5 zeolites ofvarious proveniences were investigated in a broad region ofSi/Al ratio with respect to

    the distribution ofAl atoms in the framework. The analysis of the distribution of framework Al atoms

    was done by using strictly defined conditions ofCo(II) ion exchange and UVVis, 27Al and 29Si (CP) MAS

    NMRexperiments. Evidence has been found that the distribution offramework Al atoms in ZSM-5, and

    in Si-rich zeolites in general, is not random and is not controlled by statistics, but occurs between the

    most populated Al pairs (AlSiSiAl sequences in 6MRs) and single far distant Al atoms (AlSin>2Al

    sequences) located in different rings. Depending on the type of Si- and Al-reactants and presence of

    TPA+/Na+ ingels, a broaddistribution ofAl atoms(from5 to 85%ofAl atoms inAl pairs) for Si/Al 1220can

    be achieved. At Si/Al >20, the population ofAl pairs decreases, but 90% ofsingle Al atoms can be obtained

    in the whole range ofSi/Al compositions. The local negative charge ofthe framework governed by the

    distribution of framework Al atoms inevitably controls the structure of the counter metal ion species,

    which is reflected in the catalytic properties ofmetallo-zeolites in redox reactions requiring different

    types ofcounter ion species. A high population ofAl pairs in the framework is required for stabilization

    ofdivalentbareCu(II),Co(II)and Fe(II) ionsboth inZSM-5and thebetazeolite, representing the active sites

    forC10H22-SCR-NOx,CH4-andC3H8-SCR-NOx, and forN2Odecomposition, respectively. Incontrast, singleAl atoms charge-balance monovalent cations, metal-oxo or bridged metal-oxo(hydroxo) species, the

    active sites forNOdecomposition (Cu(I) in ZSM-5and BEA*), forNH3-SCR-NOx toN2 andNO-NO2 reaction

    (Fe(III)-oxo species in ZSM-5) and C3H8-SCR-NOx/H2O (Co(II)-oxo in BEA*) in the presence of a large

    excess ofwater existing in real exhaust gases. Itis concluded that control ofthe distribution ofAl atoms

    in the framework byhydrothermal synthesis ofSi-rich zeolites could achieve the high concentration ofan

    appropriate active structure ofcountermetal-ion species required for a specified reaction andconditions.

    Thus, in addition to the usually reported total concentration ofAl atoms, the distribution ofAl atoms in

    the framework, i.e. the local negative framework charge, is a parameterwhich should be included in the

    characteristics ofSi-rich zeolites.

    2013 The Authors. Published by Elsevier B.V. All rights reserved.

    1. Introduction

    Stabilization of thecounter ionspecies asprotons and/ormono-

    andpolyvalentcations,and theirmetal-oxospeciesinside adefined

    microporevolumeby thenegative charge of the crystallinealumi-

    nosilicate framework predeterminesH- andmetallo-zeolites to act

    This is an open-access articledistributed under the terms of theCreative Com-

    mons Attribution-NonCommercial-No Derivative Works License, which permits

    non-commercial use, distribution, and reproduction in anymedium, provided the

    original authorand source arecredited. Corresponding author.

    E-mail address: [email protected](Z. Sobalik).

    as efficient and highly selective catalysts for oil and hydrocarbon

    processing, forselectivehydrocarbonoxidation, thedecompositionandreduction of nitrogen oxides in environmentprotection andin

    fine chemicals synthesis. Si-rich zeolites of ZSM-5, ferrierite, mor-

    denite and the beta zeolite structures (MFI, FER, MORand BEA*,

    respectively) have attracted great attention, because of the low

    aluminum concentration in the framework (Si/Al> 8) leading to

    strong acidity of the protons (see, e.g. Ref. [1]) and unusual redox

    and catalytic behavior of transition metal ion species (see, e.g.

    Refs. [213]), as well as shape selective effects of their microp-

    ores.

    Theoverall concentration of Al atoms in the frameworkand the

    related concentration of protons and/or cations and oxo-cations

    0926-860X/$ seefrontmatter 2013 The Authors. Published by Elsevier B.V. All rights reserved.

    http://dx.doi.org/10.1016/j.apcata.2013.07.033

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://www.sciencedirect.com/science/journal/0926860Xhttp://www.elsevier.com/locate/apcatamailto:[email protected]://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033mailto:[email protected]://www.elsevier.com/locate/apcatahttp://www.sciencedirect.com/science/journal/0926860Xhttp://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    2/8

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    3/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    Z. Sobalik et al. / Applied Catalysis A: Generalxxx (2013) xxxxxx 3

    Fig. 1. Effect of thelocal arrangement of Al atoms in theframework of ZSM-5 on theexchangeof Co(II)-complexes andbonding of Co(II)ions in dehydrated zeolites.

    Alunpair= 2x[Co(II)(H2O)6)]2+

    max 2xCo(II)bare (3)

    [AlFR] = [Alpair] + [Alunpair] + [Alsingle] (4)

    where [Co(II)(H2O)6]2+

    max is the Co(II) ion-exchange capacity of

    [Co(II)(H2O)6]2+ ions, Co(II)bare is the concentration of bare Co(II)

    in dehydrated zeolites, Co(II),, are concentrations of Co(II) ions

    in,and cationicsites, [Alpair]istheconcentrationofAlatomsin

    theAlSiSiAlsequencein one(6MR)ringof cationicsite, [Alunpair]is the concentration of close Al atoms located in different rings,

    [Alsingle] is the concentration of single far-distant Al atoms, and

    [AlFR] is the total concentration of Al in the framework.

    For ZSM-5 zeolites with framework Si/Al 1240 compositions

    analyzedso far, theconcentration of bare Co(II) ions in dehydrated

    zeolites was equal (within 5% error) to the [Co(II)(H2O)6]2+ ion-

    exchange capacity. Similarly, the concentration of Alunpair, where

    Co-oxospecies were observed in theUVspectra, didnot exceed3%

    of total Al present in the zeolite.

    To obtain a correct analysis of the Al distribution in the frame-

    work, the exclusive exchange of [Co(II)(H2O)6]2+ complexes into a

    zeolite without their hydrolysis must be guaranteed. Based on the

    extensiveexperimentalexperience[45] andseeRef.[37], thiscould

    be satisfied by carrying out the ion exchange from dilute aque-ous solutions 0.05M of Co(NO3)2 under mildly acidic conditions

    (6> pH> 5)at RT intotheNa-formofthezeolite. The accuracyof the

    estimation of the concentration of [Co(II)(H2O)6]2+ complexes in

    hydrated zeolites depends on Co concentration. It varies between

    2% for Al rich (Si/Al< 10) zeolites with large portion of Al pairs

    (Co/Al> 0.3) and 1015% for zeolites with low concentration of Al

    pairs (Si/Al 2540, Co/Al< 0.25).

    The exclusive presence of [Co(II)(H2O)6]2+ complexes in the

    solution and inside the Co-exchanged zeolite can be monitored

    by Vis spectroscopy by a typical spectrum of the strictly octahe-

    dral Co(II) complex shown in Fig. 2. All conceivable changes in

    the environmentof theCo(II) ionthe octahedral hexaquo-complex

    (e.g. formation of [Co(II)(H2O)5X]+ or Co(II) oligomeric species)

    would result in breaking down of the symmetry of this complex

    reflected in the formation of new spectroscopic species [44,46].

    The change of the spectrum of the Co(II)-exchanged zeolite due

    to the presence of an additional Co(II) complex to [Co(II)(H2O)6]2+,

    i.e. [Co(II)(H2O)5OH]+, is demonstrated in Fig. 2, where the spec-

    tra of Co-ZSM-5 prepared by the ion exchange with Co(II) nitrate

    and Co(II) acetate are compared. The Co(II) exchange into the Na-

    zeolite guarantees attainment of themaximumexchange leveldue

    to faster ion exchange into the Na- compared to H-zeolites. Na-

    formof azeolitealsoprevents formationofanynitrogen-containingCo(II)complexesthatcouldbeformedduringtheCo(II)-exchange, if

    itwouldbedonewithNH4-zeolites.Reproducibilityof thedetermi-

    nationof theexchangecapacityof [Co(II)(H2O)6]2+ ionswaswithin

    5 rel.%, i.e. within the error of chemical analysis, as revealed from

    seriesof experiments done with Na-ZSM-5 samples of Si/Al 12 and

    22.

    Fig. 2. Normalized Visspectra of theas prepared hydrated Co-ZSM-5, Si/Al 14.1.

    Sample with Co/Al 0.41 prepared by equilibration with Co(NO3)2 at RT (), and

    Co/Al 0.54 prepared by ionexchange from Co(acetate)2 at80

    C (- - -).

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    4/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    4 Z. Sobalik et al. / Applied CatalysisA: Generalxxx (2013) xxxxxx

    Fig. 3. Concentration of Al atoms in Al pairs in commercial ZSM-5 zeolites (), and

    statistical prediction of their maximum () and minimum (- - -) concentration in

    6MRs according to Ref. [24].

    Theanalysisof the distributionof frameworkAlatoms inSi-rich

    zeolitesconcludedoccurrenceof twodominantSiAlarrangements

    intheframeworkofZSM-5zeolites,andin Si-richzeolitesgenerally,which are represented by (i) the AlSiSiAl sequences (Al pairs)

    located in 6MRs enabling to balance bare divalent cations in dehy-

    dratedzeolites,and (ii) the fardistant single Al atoms inAlSin>2Al

    sequences located in different rings not providing coordination of

    a divalent cation, butwith potential to chargebalancemonovalent

    species.

    3. ZSM-5 zeolite samples

    ZSM-5 zeolites analyzed here included products of several

    industrial producers, i.e. Conteca, ALSI-PENTA, Tosoh, SdChemie

    and PQ Corporation with Si/Al ranging from 12 to 45. The identity

    and crystallinity of these samples was generally checked by XRD,

    and their pore volumes corresponded to well-developed ZSM-5structures. Chemical analysis and the 27Aland 29SiMASNMRspec-

    traindicatedhighproportionof Td-coordinatedAl intheframework

    and 12), the AlSiSiAl

    sequences(Alpairs) locatedin 6MRs,andsinglefar-distantAlatoms

    in AlSin>2Al sequences. The concentration of close Al atoms in

    different rings (Alunpair) was below 5%of total Al.

    4. Distribution of the framework Al atoms in commercial

    ZSM-5

    The concentrations of Al atoms in Al pairs (AlSiSiAl

    sequences in 6MRs) found in commercial samples with differ-

    ent Si/Al ratios are given in Fig. 3. Obviously, a general trend in

    Fig. 4. Variability of the concentration of Al atoms in Al pairs using hydrothermal

    synthesesaccording to Ref. [22] (), Ref. [21] (), Ref. [33] () and Ref. [45] ().

    decreasing relative concentrations of Al atoms accommodated in

    Al pairs with decreasing total Al concentration in the framework

    is observed, with a sharp decrease in the range of Si/Al 1220.

    Nevertheless, this tendency displays large differences in the actualconcentrations of Al atoms in Al pairs for samples with close Si/Al

    composition up to ca 20 rel.%, i.e. highly exceeding the accuracy

    of determination of the distribution of frameworkAl atoms (5%).

    Thepopulations of Al pairs predictedby using a simplistic statisti-

    cal approach arealso summarized in Fig. 3 dependingon Si/Al. The

    results of statisticalcalculationsofRiceet al. [24] areshownby lines

    depicting the concentration of Al atoms in the Al pairs under the

    conditions of applicationof the Lowensteinrule and therestriction

    for location of Al pairs only in 6MRs. Thus the lines given in Fig. 3

    excluded sites with two Al atoms in 5MRrings, in agreementwith

    our 29Si MAS NMRobservation revealing the absence of AlSiAl

    sequences in ZSM-5 of Si/Al >12. The clear discrepancy between

    the experimental results and the statistical calculations should be

    regarded as being a result of direct practical relevance showingthat the concentrations of Al pairs for the individual commercial

    samples donot followtheexpected simplestatistics. Dramatic dif-

    ferences between the distributions of Al atoms found for samples

    with close Al content in the framework represent additional sup-

    port for thepreviousconclusion on thenon-randomdistributionof

    Al atoms in ZSM-5zeolites not controlled by statistical rules. These

    differences observed for commercial ZSM-5 indicate that the Si/Al

    compositionisnotthesingleparametercontrollingthedistribution

    of Al atoms.

    5. Variability in the distribution of framework Al atoms in

    ZSM-5 caused by hydrothermal synthesis conditions

    Hydrothermal laboratory syntheses of ZSM-5 zeolites carriedout in the presenceofa template (TPAOH)andusingvariousSi-and

    Al-reactants,Si/Al gelcompositions,andin thepresence/absenceof

    Na+ ions (details reported in Refs. [2022,33,34,45]) led to a high

    variability in the distribution of Al atoms in the framework over

    a wide range of Si/Al compositions (Fig. 4). For Si/Al 1215 in the

    products the concentrations of Al atoms in Al pairs could be tuned

    from5 to 85% by changing the composition of the reactants.While

    a highly predominant concentration of single Al atoms could be

    obtained ina widerange ofSi/Al from12to 45, the chanceto incor-

    porate Al pairs obviouslydecreaseswithdecreasing concentration

    of frameworkAl atoms.

    Fig. 5 depicts sets of hydrothermal syntheses carried out with

    various reactants (Al chloride vs. Al nitrate; TEOS vs. Na-silicate

    vs. Si-Al precursor) under the same (volume, T, Si/TPAOH 2.8)

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    5/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    Z. Sobalik et al. / Applied Catalysis A: Generalxxx (2013) xxxxxx 5

    Fig. 5. Effect of Si/Al on the concentration of Al atoms in Al pairs in ZSM-5 zeolite

    for hydrothermal syntheses using: Al chloride+ TEOS (), Si-Al precursor (), Al

    nitrate +TEOS (), Al nitrate+ Na silicate (); according to Refs. [33,32].

    conditions of hydrothermal synthesis. It was shown that the use

    of Al nitrate and Na-silicate in the gel strongly supports the

    incorporation of single Al atoms into the framework, while theSiAl precursor and AlCl3/TEOS yield a higher population of Al

    pairs. Moreover, while the gel containing the SiAl precursor or

    AlCl3/TEOS exhibited a decrease in the concentration of Al pairs

    with increasing Si/Al ratio, quite the opposite trend was obtained

    withAlCl3/TEOS gels. A markedeffectof Si/Al was not observed for

    ZSM-5 products with low population of Al pairs and high popula-

    tion of single Al atoms (90% of total Al). These findings strongly

    support the suggestion of the decisive role of the type of reactants

    on the distribution of Al atoms in the framework of ZSM-5 zeo-

    lites, and further contradict the assumption about the random or

    statistical distributionof frameworkAl atoms.

    Analysisof themechanismbehind thehydrothermalZSM-5syn-

    thesis leading to incorporation of Al pairs vs. single Al atoms in

    the framework and understanding of the function of the individ-ual reactants are beyond the scope of this paper. We have already

    suggestedthat the polarizationof TPA+ by anions andthe presence

    of Na+ ions play a decisive role in the arrangement of the Al atoms

    in SiAl sequences during the first stages of the interactions in the

    gel. For details on the 29Si, 27Al and 13C MAS NMR study of the

    gel composition and corresponding distributionof Al atoms in the

    framework of ZSM-5 products, the reader is referred to the recent

    paper of Dedecek et al. [33].

    6. Impact of the distribution of framework Al atoms on

    catalytic NOx processes over metallo-zeolites

    Obviously, the structure of the resulting counter-ion species in

    Si-rich zeolites obtained by ion exchange (in both aqueous andgaseous (CVD) environment) is controlled by both the counter

    parts, i.e. the type of metal ion complex and the local nega-

    tive charges occurring in the framework and governed by the

    presence of Al pairs and single Al atoms. While the exchanged

    [M(II)(H2O)6]2+ complexes in zeolites are predominantly balanced

    by Al pairs, the negative charge of single Al atoms is sufficient for

    monovalent [M(II)(H2O)5X]+ entities. After zeolite dehydration,

    the Al pairs in 6MRs strongly stabilize bare divalent cations coor-

    dinated to the framework oxygen atoms (see Fig. 1). At the same

    time,monovalent species adjacent to singleAl atoms (monovalent

    cationsormetal-oxo(hydroxo) ions), or bridgedmetal-oxospecies,

    charge-balanced by two single Al atoms in different rings, can be

    formed. An analogous (but more complex) situation, necessarily

    considering the total positive charge of the metal complex, exists

    Fig. 6. Effect of Cu loading in Cu-ZSM-5 on TOF in C10H22-SCR-NO under water

    presence at 250C and inNOdecomposition at 400 C (seeRef. [51]).

    for the location and charge balance of oxo(hydroxo) complexes of

    trivalent cations.

    Theobjective of this paper is nota detailedanalysis of thestruc-ture of various counter species, but rather to evaluate the effect

    of the distribution of Al atoms in the framework on the activity of

    the counter-ion species in Si-rich zeolites in redox reactions stud-

    ied in our laboratory. This effect is outlined on the Cu-, Fe- and

    Co-zeolites of ZSM-5 and beta structures with various distribu-

    tions of Al atoms in the framework, and their activity in NO and

    N2O decomposition, in oxidation of NO to NO2 and SCR-NOx by

    methane, propane, decane or ammonia,moreover, in the presence

    and absence ofwater vapor in the feed.

    6.1. Cu-ZSM-5 and Cu-BEA*

    While the ion exchange from aqueous Cu(II) nitrate solutions

    preferablyoccurs through [Cu(II)(H2O)6]2+, theionexchange usingCu acetate solutions also includes [Cu(II)(H2O)5X

    ]+ complexes,

    exchanged particularly intothehighly-loadedCu-ZSM-5. First, and

    preferably at low loadings, the Cu(II) ions adjacent to the Al pairs

    in 6MRs of cationic sites are exchanged, followed by introduc-

    tion of [Cu(II)X]+ complexes charge-balanced mostly by single

    Al atoms. In the dehydrated samples, the bare Cu(II) ions (orig-

    inated from [Cu(II)(H2O)6]2+) are not easily reduced compared

    to [Cu(II)(H2O)5X]+ transformed into [Cu(II)OH]+ or dinuclear

    [Cu(II)-O-Cu(II)]2+ bothreadilyreduced toCu(I),whichsurviveeven

    in oxygen atmosphere at elevated temperatures [3,4,47]. These

    conclusions are based on the blue-shift in the UV-Vis spectrum of

    theCu(II) aquocomplexes,and characteristic luminescencespectra

    of bare Cu(I) ions, IR spectra of Cu(II)NO complexes [48,49], and

    their redox properties in dehydrated Cu-zeolites [49,50].The TOF per Cu atom of NO decomposition over Cu-ZSM-5

    clearly increaseswithincreasingCu/Alconcentrations (asobserved

    in many laboratories) similar to the increasing population of Cu

    species adjacent to single Al atoms (Fig. 6, data from Refs. [4,51]).

    Accordingly, the active sites in NO decomposition represent the

    generallyacceptedCu(I) ions,which areadjacenttosingleAlatoms,

    more populated in the highly loaded Cu-zeolites. Similar high

    activity inNOdecomposition (inTOF perCu)of the Cu ions charge-

    balanced by single Al atoms and reflected in the shift of the high

    energy edgeof the Cu(II) Vis band in the spectrumof hydrated Cu-

    zeolite was observed and is depicted in Fig. 7 (data given in Ref.

    [52]).

    In contrast, the rateof the C10H22-SCR-NOx/H2O reaction in the

    presence of water (12%) over Cu-ZSM-5 sharply decreases with

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    6/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    6 Z. Sobalik et al. / Applied CatalysisA: Generalxxx (2013) xxxxxx

    Fig. 7. The effect of the position of high energy edge of the Cu(II) Vis band ofmax-

    imum loaded hydrated Cu-BEA* samples prepared from different parents on the

    conversion of NO perCu forNO decomposition (see Ref. [52]).

    Fig. 8. Effect of Co loading on the yield of N2 in C3H8-SCR-NOx over Co-BEA-I ()

    with prevailing concentration of single Al atoms (Si/Al 15.6, Alsingle0.59mmolg1,

    61%), and Co-BEA-II () with lower concentration of single Al atoms (Si/Al 11.7,

    Alsingle 0.41mmol g1, 34%). Maximum concentrations of bare Co(II) ions balanced

    by Al pairs are indicated forCo-BEA zeolites by arrows. Data taken from Ref. [60].

    Cu-loading (Fig. 6, for details see Ref. [51]). This indicates that, in

    this reaction, the most active sites represent the Cu(II) ions bal-

    anced by Al pairs. With the SCR-NOx reaction the redox process

    requires divalent Cu(II) as the active site with participation of the

    Cu(II)/Cu(I) redox cycle. However, the presence of water vapor is

    knowntobedetrimental for the open coordination sphereof Cu(II)

    ions balancedby Al pairs. Nevertheless, in this reaction carried outat250 C a strong adsorption of predominantly of olefinic products

    of decane cracking and of NO2 on Cu(II) occurs, preventing water

    adsorption.

    6.2. Fe-ZSM-5

    Fe ion exchange into ZSM-5 is very complex. In aqueous solu-

    tions of Fe salts of both Fe(II) and Fe(III) ions substantial hydrolysis

    takesplace [37]. In the procedureusing chemicalvapor deposition

    from FeCl3, the FeCl2+ and FeCl2+ species are exchanged with fol-

    lowing their hydrolysis. Various procedures employed for Fe ion

    exchange led in dehydrated Fe-ZSM-5 (even in oxidizing atmo-

    sphere) at lowFe loadings(Fe/Al

  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    7/8

    http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0145http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0140http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0135http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0130http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0125http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0120http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0115http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0110http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0105http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0100http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0095http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0090http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0085http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0080http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0075http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0070http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0065http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0060http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0055http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0050http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0045http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0040http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0035http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0030http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0025http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0020http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0015http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0010http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0005http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033
  • 7/30/2019 1-s2.0-S0926860X13004432-main (1)

    8/8Please cite this article in press as: Z. Sobalik, et al., Appl. Catal. A: Gen. (2013), http://dx.doi.org/10.1016/j.apcata.2013.07.033

    ARTICLE IN PRESSGModel

    APCATA-14350; No.of Pages8

    8 Z. Sobalik et al. / Applied CatalysisA: Generalxxx (2013) xxxxxx

    [30] J. Dedecek, D. Kaucky, B. Wichterlova, O. Gonsiorova, Phys. Chem. Chem. Phys.4 (2002)54065413.

    [31] O.H.Han,C.S.Kim,S.B. Hong, Angew. Chem. Int. Ed. 41 (2002) 469472.[32] O.Bortnovsky,O. Tokarova,B.Wichterlova,J. Dedecek,Z. Sobalik,O. Gonsiorova,

    V. Balgova, (PatentWO2011095140).[33] J. Dedecek, V. Balgova, V. Pashkova, P. Klein, B. Wichterlova, Chem. Mater. 24

    (2012)32313239.[34] V. Gabova, J. Dedecek, J. Cejka, Chem. Commun. (2003) 11961197.[35] P. Sazama, J. Dedecek, V. Gabova, B. Wichterlova, G. Spoto, S. Bordiga, J. Catal.

    254 (2008) 180189.[36] Z. Sobalik, J. Novakova,J. Dedecek, N.K. Sathu,E. Tabor,P. Sazama, P. Stastny, B.

    Wichterlova, Micropor.Mesopor.Mater. 146 (2011) 172183.[37] C.F. Baes, R.E. Mesmer, TheHydrolysis of Cations,Wiley,New York, 1976.[38] N. Katada, T. Kanai, M. Niwa, Micropor.Mesopor. Mater. 75 (2004) 6167.[39] T.I. Koranyi, J.B. Nagy, J. Phys. Chem. B 109 (2005) 1579115797.[40] S. Kuriyavar, O. Bortnovsky, Z. Tvaruzkova, Z. Sobalik, Collect. Czech. Chem.

    Commun. 66 (2001) 685692.[41] J. Dedecek,D. Kaucky, B.Wichterlova,Micropor.Mesopor.Mater. 3536 (2000)

    483494.[42] J. Dedecek, J. Cejka, M. Oberlinger, S. Ernst, Stud. Surf. Sci. Catal. 142 (2002)

    2330.[43] L. Benco, T. Bucko, J. Hafner, H. Toulhoat, J. Phys. Chem. B 109 (2005)

    2036120369.[44] J. Dedecek, L. Capek, D. Kaucky, Z. Sobalik, B. Wichterlova, J. Catal. 211 (2002)

    198207.

    [45] V.Gabova, PhDThesis,J. HeyrovskyInstitute of Physical Chemistryof theASCR(2004).

    [46] D. Kaucky, J.I. Dedecek, B. Wichterlova, Micropor. Mesopor. Mater. 31 (1999)7587.

    [47] Y. Kuroda, M. Iwamoto, Top. Catal. 28 (2004) 111118.[48] J. Dedecek, B. Wichterlova, J. Phys. Chem. B 101 (1997) 1023310240.[49] J. Dedecek, Z. Sobalik, Z. Tvaruzkova, D. Kaucky, B. Wichterlova, J. Phys. Chem.

    99 (1995)1632716337.[50] R. Bulanek, B.Wichterlova,Z. Sobalik, J. Tichy,Appl.Catal. B-Environ. 31 (2001)

    1325.[51] J. Dedecek, L. Capek, B. Wichterlova, Appl. Catal. A-Gen. 307 (2006) 156164.

    [52] J. Dedecek, O. Bortnovsky, A. Vondrova, B. Wichterlova, J. Catal. 200 (2001)160170.

    [53] P. Sazama, N.K. Sathu, E. Tabor, B. Wichterlova, S. Sklenak, Z. Sobalik, J. Catal.299 (2013) 188203.

    [54] K. Jisa, J. Novakova, M. Schwarze, A. Vondrova, S. Sklenak, Z. Sobalik, J. Catal.262(2009) 2734.

    [55] E. Tabor, K. Zaveta, N.K. Sathu, A. Vondrova, P. Sazama, Z. Sobalik, Catal. Today175 (2011) 238244.

    [56] D.Kaucky,A.Vondrova,J. Dedecek,B. Wichterlova,J. Catal.194 (2000) 318329.[57] J.N. Armor, Catal. Today 26 (1995) 147158.[58] A.W. Aylor, L.J. Lobree, J.A. Reimer, A.T. Bell, Stud. Surf. Sci. Catal. 101 (1996)

    661670.[59] L. Capek, J. Dedecek, B.Wichterlova, J. Catal. 227 (2004) 352366.[60] L. Capek, J. Dedecek, P. Sazama, B.Wichterlova, J. Catal. 272 (2010) 4454.

    http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0300http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0295http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0290http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0285http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0280http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0275http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0270http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0265http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0260http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0255http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0250http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0245http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0240http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0235http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0230http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0220http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0215http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0210http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0205http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0200http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0195http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0190http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0185http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0180http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0175http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0170http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0165http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0155http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://refhub.elsevier.com/S0926-860X(13)00443-2/sbref0150http://localhost/var/www/apps/conversion/tmp/scratch_7/dx.doi.org/10.1016/j.apcata.2013.07.033