METABOLISM OF TOXIC METALS IN INDUSTRIAL SYMBIOSIS IN THE CEMENT INDUSTRY – A GLOBAL

REVIEW AND ANALYSIS

Stegemann, J.A.1, Zhang, W.S. 2, Wang, Z.Y.2, Wei, J.X.3, Yu, Q.J. 3, and Zhou, Q. 1

1Centre for Resource Efficiency & the Environment, Department of Civil, Environmental & Geomatic

Engineering, University College London, UK

2China Building Materials Academy, Beijing, China

3South China University of Technology, Guangzhou, China

Abstract

UNDER CONSTRUCTION

1 Introduction

Over the past three decades, the concept of industrial ecology has emerged as central to the

development of resource efficiency and sustainability (e.g., Frosch & Gallopoulos, 1989; Chertow,

2000). With its comparable need to make efficient use of resources, industrial activity is analogous

to a natural ecosystem, where a network of companies (organisms) must innovate (adapt) in

response to market (environmental) pressures, and competition leads to survival of the fittest. In a

natural ecosystem, resources are shared and cycled between members for mutual benefit in

symbiotic relationships. In industrial symbiosis, the by-products of one industry become the raw

materials for another.

Concrete is the most widely used material in the world and essential to much of our infrastructure.

As well as consuming about 11% of global industrial energy, cement production consumed more

than 5 Gt of non-fuel raw materials in 2011. More efficient management of the significant

proportion of global resources consumed by the cement/ concrete industry is therefore important to

sustainability. As obtaining energy and materials resources at lower cost has always been good

business, industrial symbiosis has occurred in the cement industry since long before the

popularisation of industrial ecology. The most common practices have been: 1) co-processing of

alternative fuels and raw materials (ARF), whereby a) wastes with high calorific value replace fossil

fuels, and/or b) mineral wastes replace raw material feeds (limestone, clay and supplements), to the

cement kiln, and 2) replacement of Portland cement clinker with pozzolanic wastes and diluents to

produce blended cements. Minerals waste may also replace natural aggregate in concrete

(Stegemann, 2014).

Many wastes contain elements or compounds that have the potential to interfere with cement

chemistry or pollute the environment and the viability of utilising wastes in cement production

requires that: 1) the manufacturing process is not adversely affected or can be adapted, 2) the

technical characteristics of the final cementitious material are appropriate to its intended use, and 3)

the risks of negative impacts on health or the environment from manufacturing and use of the

cementitious material are unchanged or reduced (Stegemann, 2014). In general, there has been a

high degree of conservatism and regulatory influence regarding the industrial by-products that are

allowed to enter the cement production system, and the cement industry has promoted industrial

symbiosis as a safe practice (e.g., Cembureau, 1997). However, when resources are more scarce and

costly and waste builds up in an ecosystem at levels that are detrimental to its health, there is a

greater incentive to evolve more efficient by-product utilisation in more specialised industrial-

ecological niches. Consequently, there is increasing pressure for a wider range of waste types,

including hazardous wastes, to be used in cement-based products.

The objectives of this review are therefore to:

1) to examine our present understanding of the fate and behaviour of heavy metals in co-

processing, through the cement kiln, into clinker and air pollution control dusts, to hydrated

Portland and blended cement pastes and the environment, and

2) identify areas where further research is needed to enable resource efficiency with concomitant

protection of the environment from heavy metal pollution.

2 Approach

Review of the literature focussed on …

(Achternbosch et al., 2003, 2005; Adaska & Taubert, 2008; Alp, Deveci, Yazici, Türk, & Süngün, 2009;

Alp, Deveci, & Süngün, 2008; Andrade, Maringolo, & Kihara, 2003; Aouad, Laboudigue, Gineys, & NE,

2012; Artelt & Greinacher, 1993; a M. Barros, Tenório, & Espinosa, 2002; A. M. Barros, Espinosa, &

Tenório, 2004; A. M. Barros, Tenório, & Espinosa, 2004; Basten et al., 2002; Battelle/WBCSD, 2002;

Benard et al., 2009; Bermudez, Jasan, Plá, & Pignata, 2012; Bernardo, Marroccoli, Nobili, Telesca, &

Valenti, 2007; Bochenek & Kurdowski, 2013; Bodaghpour, Joo, & Ahmadi, 2012; Bolio-Arceo &

Glasser, 1998, 2000; I Bonhoure, Wieland, Scheidegger, & Tits, 2002; I. Bonhoure, Scheidegger,

Wieland, & Dähn, 2002; Isabelle Bonhoure, Baur, Wieland, Johnson, & Scheidegger, 2006; Isabelle

Bonhoure, Wieland, Scheidegger, Ochs, & Kunz, 2003; BUWAL, 1998; Carrasco, Bredin, Gningue, &

Heitz, 1998; Cembureau, 1997, 2009; Q. Y. Chen et al., 2007; Y.-L. Chen et al., 2009; Y.-L. Chen,

Chang, Lai, & Ko, 2012; Chen, Jida; Liao, Shiguo; Xie, Bin; Zhang, Liwei; Wang & Jiang, 2011; Chertow,

2000; Chinyama, 2011; CPCB, 2010; Dąbkowska- Naskręt, Jaworska, & Długosz, 2014; Degré, 2006;

Dekeukelaere, 2011; Dell’Orso, Mangialardi, Evangelista Paolini, & Piga, 2012; Eckert, Guo, &

Moscati, 1999; Eckert & Guo, 1998; Ekincioglu, Gurgun, Engin, Tarhan, & Kumbaracibasi, 2013; El-

Awady & Sami, 1997; Environment Agency, 2008; D C R Espinosa & Tenorio, 2001; Denise C R

Espinosa & Tenorio, 2000; FIERENS & VERHAEGE.JP, 1971; Frosch & Gallopoulos, 1989; Gaona, Dähn,

Tits, Scheinost, & Wieland, 2011a, 2011b; Gaona, Kulik, Macé, & Wieland, 2012; Gaona, Wieland,

Tits, Scheinost, & Dähn, 2013; Genon & Brizio, 2008; Gheorghe, Radu, Stac, & Saca, 2013;

Giannopoulos, Kolaitis, Togkalidou, Skevis, & Founti, 2007; Gierzatowicz, 2000; Gineys, Aouad, &

Damidot, 2010; Gineys, Aouad, Sorrentino, & Damidot, 2012; Gineys, Aouad, & Damidot, 2011;

Gineys, Aouad, Sorrentino, & Damidot, 2011; Gomes, Drumond, Neto, & Lira, 2013; Guan, Zhang,

Yang, & Yang, 1998; Guo & Eckert, 1996; Guo, 1997; Hanna et al., 1995; Hasanbeigi, Lu, Williams, &

Price, 2012; Heimburg, 1981; Hekal, Kishar, Hegazi, & Mohamed, 2011; Hill & Sharp, 2003;

HOLCIM/GTZ, 2006; Hsiao, Wang, & Yang, 2001; Huang, Yang, & Wang, 2012; Ivey et al., 1990; Jones,

Bankiewicz, & Hupa, 2014; Kaddatz, Rasul, & Rahman, 2013; Kapur & Kapur, 2004; Karagiannis &

Ftikos, 2012; Karstensen, 2007, 2008; Kikuchi, 2001; KIRCHNER, 1985, 1986, 1987; Klein & Hoenig,

2004; Kleppinger, 1993; Kolovos, Barafaka, Kakali, & Tsivilis, 2005; Krammart & Tangtermsirikul,

2004; KRCMAR, LINNER, & WEISWEILER, 1994; Lam, Barford, & McKay, 2011; Li, 2013a, 2013b;

Lieber & Gebauer, 1969; S. Lin, Su, & Tong, 2007; Y.-M. Lin, Zhou, Zhou, & Wu, 2011; Lin, Yi-Ming;

Zhou, Shao-qi; Zhou, De-jun; Wu, 2011; Ling, Jin, & Nie, 2008; Liu & Wang, 2011; Lorea, 2007; B. G.

Ma, 2009; X.-W. Ma, Chen, & Wang, 2010; Madlool, Saidur, Hossain, & Rahim, 2011; Martens,

Jacques, Van Gerven, Wang, & Mallants, 2010; Medina, Borunda, & Elguézabal, 2006; Mokrzycki &

Uliasz-Bochenczyk, 2003; Murat & Sorrentino, 1996; Murray & Price, 2008; Napia, Sinsiri,

Jaturapitakkul, & Chindaprasirt, 2012; Navia, Rivela, Lorber, & Méndez, 2006; Ogunbileje et al., 2013;

Pan, Huang, Kuo, & Lin, 2008; Paone, 2008; Park, 2000; PCA, 1992; Pembina Institute, 2005; Peng,

Zheng; Yu, Li-feng; Ding, Qiong; Wang, Kai-xiang; Gao, 2012; Pinakidou et al., 2006; Polat, Gürol,

Budak, Karabulut, & Ertuǧrul, 2004; Prodjosantoso & Kennedy, 2003; Pudasainee et al., 2009; Puntke

& Schneider, 2001; Qiao, Poon, & Cheeseman, 2007; Qiu, Luo, Shi, & Ni, 2011; Ract, Espinosa, &

Tenório, 2003; Reijnders, 2008; Romano & Rodrigues, 2008; Saikia, Kato, & Kojima, 2007; a M.

Scheidegger et al., 2006; A M Scheidegger et al., 2006a, 2006b; André M. Scheidegger et al., 2001,

2006; André M. Scheidegger, Wieland, Scheinost, Dähn, & Spieler, 2000; Schneider & Kuhlmann,

1997; Schuhmacher, Nadal, & Domingo, 2009; Serclerat, Massardier, Moszkowicz, & Murat, 1997;

Serclerat, Moszkowicz, & Murat, 1997; Serclérat, Moszkowicz, & Pollet, 2000; Serclérat &

Moszkowicz, 1997; Seyler, Hellweg, Monteil, & Hungerbühler, 2005; Shih, Chang, & Chiang, 2003;

Shih, Chang, Lu, & Chiang, 2005; Sikalidis, Zabaniotou, & Famellos, 2002; Sinyoung, Asavapisit,

Kajitvichyanukul, & Songsiriritthigul, 2011; Sinyoung, Songsiriritthigul, Asavapisit, & Kajitvichyanukul,

2011; SPRUNG, KIRCHNER, & RECHENBERG, 1984; SPRUNG, RECHENBERG, & BACHMANN, 1994;

SPRUNG & RECHENBERG, 1978, 1983, 1994; SPRUNG, 1992; Sreekrishnavilasam, King, & Santagata,

2006; Stegemann, 2014; Stephan, Knofel, & Hardtl, 2001; Stephan, Maleki, Knöfel, Eber, & Härdtl,

1999a, 1999b; Stephan, Mallmann, Knöfel, & Härdtl, 2000a, 2000b; Sun, Bai, Man, Jiang, & Shen,

2007; Taeb & Faghighi, 2002; Tamas & Abonyi, 2002; Thomanetz, 2012; M A Trezza & Scian, 2000,

2007; Monica Adriana Trezza & Scian, 2009; Tsakiridis, Agatzini-Leonardou, & Oustadakis, 2004;

Tsakiridis, Papadimitriou, Tsivilis, & Koroneos, 2008; Tsiliyannis, 2012; UNEP, 2012; H. . van der Sloot,

2000; H. A. van der Sloot et al., 2011; H. van der Sloot et al., 2008; van Oss & Padovani, 2002, 2003;

VDZ, 1996, 2001, 2005, 2011; Vespa, Daehn, Wieland, Grolimund, & Scheidegger, 2006; Vespa,

Dähn, Grolimund, Wieland, & Scheidegger, 2007, 2006; Vespa, Wieland, Dähn, Grolimund, &

Scheidegger, 2007; Vespa, Wieland, Dahn, Grolimund, & Scheidegger, 2004; Vespa, Dähn, Gallucci,

et al., 2006; Vespa, Dähn, Grolimund, Harfouche, et al., 2006; L. Wang, Jin, Li, & Nie, 2010; L. Wang,

Jin, Nie, & Li, 2010; R. Wang, Chen, & Shi, 2009; Wang, Lei; Jin, Yiying;Liu, 2009; WBCSD/CSI, 2005;

WEISWEILER & KRCMAR, 1989, 1990; WEISWEILER, LINNER, & KRCMAR, 1990; Wichman, Sprenger,

Wobst, & Bahadir, 2000; Wieland, Bonhoure, Fujita, Tits, & Scheidegger, 2003; Wieland, Tits, Spieler,

Dobler, & Scheidegger, n.d.; WRAP, 2012; Wu, Shi, de Schutter, Guo, & Ye, 2012; Xin & Yang, 2005;

Xue, Yang, & Huang, 2011; Yan, Karstensen, Huang, Wang, & Cai, 2010; Y.-F. Yang, Huang, Zhang,

Yang, & Wang, 2009; Yu Yang, Yang, Huang, Zhang, & Wang, 2008; Yufei Yang, Huang, Yang, Huang,

& Wang, 2011; Yu-fei Yang, Huang, Yang, & Wang, 2008; Yufei Yang, Xue, & Huang, 2013; Yufei Yang,

Yang, Wang, & Huang, 2011; Yu, Lin, Hisada, Saeki, & Nagataki, 2002; Zemba et al., 2011; H. Zhang,

Pang, He, & Shao, 2010; J. Zhang et al., 2009; J. Zhang, Liu, Li, Nie, & Jin, 2008; T. Zhang, Gao, Gao,

Wei, & Yu, 2013; Zhu, Takaoka, Oshita, & Morisawa, 2011; Ziegler, Scheidegger, Johnson, Dähn, &

Wieland, 2001)

3 Results

3.1 Co-processing of wastes containing heavy metals in the cement kiln as alternative fuels

(Genon & Brizio, 2008; Li, 2013a; Y.-M. Lin et al., 2011; Seyler et al., 2005)

3.2 Co-processing of wastes containing heavy metals in the cement kiln as alternative raw

materials

(Alp et al., 2008, 2009; Bernardo et al., 2007; Y.-L. Chen et al., 2009, 2012; Chen, Jida; Liao, Shiguo;

Xie, Bin; Zhang, Liwei; Wang & Jiang, 2011; Denise C R Espinosa & Tenorio, 2000; Gomes et al., 2013;

Guan et al., 1998; Kapur & Kapur, 2004; Krammart & Tangtermsirikul, 2004; Lam et al., 2011; B. G.

Ma, 2009; Medina et al., 2006; Pan et al., 2008; Qiu et al., 2011; Saikia et al., 2007; Taeb & Faghighi,

2002; Monica Adriana Trezza & Scian, 2009; Tsakiridis et al., 2004, 2008; L. Wang, Jin, Nie, et al.,

2010; Wu et al., 2012; Zhu et al., 2011)

3.3 Heavy metal content of commercial cements

3.4 Fate of metals in the cement kiln

3.4.1 Volatilisation and mineralogy of gas- entrained and condensed solid phases

3.4.2 Clinker formation and mineralogy

Stephan

(Andrade et al. 2003)

Addition of 1% ZnO, Pb(NO3)2 and NH4VO3

V has shown a preferential partition towards C2S. Zn appears in higher amounts in periclase,

and C3S has higher Zn contents than C2S. Pb concentrates in minute spherules and

partitions toward C3S in small amounts

(Barros et al. 2002)

(Gineys et al. 2011)

maximum amount that could be incorporated into a standard clinker whilst reaching thelimit of solid solution of its four major phases (C3S, C2S, C3A and C4AF).

Threshold limit was considered to be reached when XRD showed new phases

The threshold limits for Cu, Ni, Zn and Sn were respectively equal to 0.35, 0.5, 0.7 and 1wt.%.

beyond the threshold limits. Ni was associated with Mg as a magnesium nickel oxide(MgNiO2) and Sn reacted with lime to form a calcium stannate (Ca2SnO4).

Cu changed the crystallisation process and affected therefore the formation of C3S. Indeed ahigh content of Cu in clinker led to the decomposition of C3S into C2S and of free lime. Zn, inturn, affected the formation of C3A. Ca6Zn3Al4O15 was formed whilst a tremendousreduction of C3A content was identified.

(Gineys et al. 2011)

The threshold limit for Sn was affected by the Bogue content in interstitial phases.

The threshold limit for Zn was affected by the Bogue content in C3S

Cu was unaffectedby any modifications of clinker composition

(Prodjosantoso & Kennedy 2003)

solubility of Mg, Cd, Pb and Ba in Ca3Al2O6

Mg cations are found to partially substitute for Ca2 +, and structural refinements show thatMg preferentially occupies the smaller six-coordinate sites in Ca3 xMgxAl2O6.

Ba preferentially occupies the larger eight- and nine-coordinate sites.

X-ray microanalysis suggests that Pb and Cd are lost from the samples during thepreparation process.

(Ract et al. 2003)

Samples were prepared by additions from 0.25 to 5 wt.% of a galvanic sludge to an industrialclinker

raw-material in a laboratory device

up to 2 wt.% of a galvanic sludge containing 2.4 wt.%Cu and 1.2 wt.% Ni to clinker raw-material do not affect the clinkeringreactions and that these metals are totally incorporatedinto the clinker.

[this is only 480 mg/kg Cu, 240 mg/kg Ni!]

3.5 Fate of metals in the hydrated paste

3.5.1 Fundamental studies

Hydrated cement paste, whether Portland or blended, is composed of highly alkaline crystalline and

amorphous phases, including calcium silicate hydrate (C-S-H, at least 50% on a dry mass basis),

Ca(OH)2 (up to 20% on a dry mass basis), as well as hydrated calciumalumino-ferrites and calcium

sulphoaluminates, including ettringite [Ca6Al2(SO4)3(OH)12.26H2O].and monosulphate

[[Ca2AlSO4(OH)6).12H2O ](e.g., Lothenbach et al. 2011). Heavy metals can be taken up into these

cement hydration products, or sorbed onto their surfaces, or form separate solid phases in the

alkaline conditions, as further discussed in an excellent review by Johnson (2002). Recent

fundamental and valuable studies in this area have also been undertaken by Wieland and co-

workers, who have used x-ray absorption spectroscopy (XAS) to study speciation of various metals

doped into C-S-H and hardened cement pastes.

It is thought that cation-exchange can occur in the CaO interlayer of C-S-H; replacement of Ca2+ by

Mg2+ has been reported (e.g., Massazza, 1998), which suggests that the potential for replacement by

other alkaline earth elements, such as Sr, exists. The crystalline calcium silicate hydrate mineral

tobermorite has been shown to have a high capacity for exchange of Ca2+ with Co2+, Ni2+, Cu2+ and

Mg2+ (Johnson 2002). However, there is good evidence that Zn and Pb are incorporated as oxides in

the silicate layers of C-S-H, rather than exchanging for Ca2+ (Ziegler et al. 2001, Tommaseo and

Kersten 2002, Rose et al. 2000).

Trivalent cations, such as Cr3+, Ni3+ and Co3+, can also substitute for Al3+ or Fe3+ in ettringite, as

reported by Gougar and co-workers (1996), and possibly other hydrated calcium aluminates such as

hydrogarnet [C3ASxH6-2x ]which has been shown to take up Cr3+ (Kindness et al., 199b). Gougar (1996)

also reviews reports that divalent cations, such as Ba2+, Cd2+, Co2+, Hg2+, Ni2+, Pb2+, Sr2+ and Zn2+, can

replace Ca2+ in ettringite minerals, but the evidence for this is not strong. As reviewed by Johnson

(2002), heavy metals that form oxyanions, such as As, Cr(VI), Mo, Sb, Se, Te, V and W can substitute

for sulphate in ettringite and monosulphate.

When the sorption or exchange capacity of cement hydration products is exceeded, metals will form

new solid phases. Due to the alkaline nature of cement hydration products, with a typical pH of

12.3, and a possible range from about 10 to 14, the most likely anion to form a metal-bearing salt is

the hydroxide ion, OH-. Metals may form single-metal hydroxides, but may also form other phases

such as calcium zincate, or other mixed hydroxides (e.g., Scheidegger et al. 2000, Johnson 2002).

Oxyanions may also precipitate with calcium (Johnson 2002)

Wieland and coworkers - significant uptake of stannate and uranate [Sn(IV) and U(VI)] by C-S-H and a

structural model of the binding mechanism has been proposed on the basis of X-ray absorption

spectroscopy studies.

An important difference between heavy metals introduced by co-processing of wastes, as compared

with those introduced by blending of mineral wastes with blended cements, is that the former are

likely to be more intimately mixed with cement phases and may have undergone a change in

speciation, whereas the latter may be associated with waste particles. However, inorganic

encapsulated particles are likely to react with the cement matrix to some degree. Depending on

reaction kinetics, soluble species such as chlorides and sulphates may dissolve during or soon after

mixing of cement powder with water, releasing metals for other interaction with the cement

hydration products, whereas species such as oxides may dissolve more gradually and participate in

secondary reactions during cement hardening and curing, and some aluminosilicates may retain

their original form in the waste in the long term.

3.5.2 Portland cement from co-processing

3.5.3 Blended cements with mineral wastes

Hsaio et al. (2001) observed respeciation of soluble CuCl2 to precipitated Cu(OH)2, and also

oxidation of Cu+ to Cu2+ in municipal waste incinerator fly ash solidified with Portland cement.

4 Leaching of metals from cement pastes

Hydrated cement paste provides a dense physical matrix of low permeability, which constitutes a

physical barrier to leaching.

AsO43- and MoO4

2- are known to form calcium salts of low solubility at high pH, whereas the solubility

of calcium salts of AsO33-, CrO4

2-, SeO32-, SeO4

2- is higher, and that of Sb and V salts is unknown

(Johnson 2002).

The measured porewater or leachate concentrations of metal contaminants are often found to be

lower than the solubilities of their hydroxide (Johnson, 2002). If the total contaminant

concentration in the product is lower than the capacity of the matrix for uptake of the contaminant,

the leachate concentration is controlled by partitioning between the solid and liquid, rather than

metal hydroxide solubility. This phenomenon is evident for Pb, whose solubility is an order of

magnitude lower than the solubility in equilibrium with hydroxide at pH 10 to 13.5, and several

orders of magnitude lower at more acidic pHs (Johnson, 2002). However, Pb remains by far the most

soluble metal in the alkaline environment provided by a cement matrix.

Based on leaching data alone, it is difficult to know the mechanism by which the matrix takes up

contaminants. It is assumed that surface sorption is responsible at lower contaminant

concentrations, and uptake into the hydration products through solid solution occurs as

contaminant concentrations increase and surface sorption sites are saturated.

5 Fate of heavy metals in demolition of cement-based structures

Achternbosch

- use of: electric arc furnace dust (EWC code 10 02 07*) as iron supplement by St Lawrence Cement,

air pollution control (APC) residues from energy-from-waste (EfW) plants, which are classified as

hazardous wastes under EWC code 19 01 07*, in cement-based products by Cenin (cenin.co.uk) and

Lignacite (www.lignacite.co.uk),; other proposals include utilisation of leaded cathode ray tube glass

(EWC code 16 02 13*/15*) ….

6 Discussion

6.1 Research Requirements

7 Conclusions

8 References [UNDER CONSTRUCTION; NEEDS SORTING AND SOME ADDITIONS, E.G., CLINKER

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