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Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED STUDIES Doctorate course in Chemical Sciences PhD thesis Cycle XX Scientific-sector CHIM/06 PhD Candidate: Dr. Melissa Paoletti Tutors: Prof. Enrico Marcantoni Dr. Gianluca Paniccià

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Page 1: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Lewis acids in the preparation of the heterocyclic compounds: synthesis

andcharacterization of the impurities of

API

2004/05 – 2006/07

SCHOOL OF ADVANCED STUDIES

Doctorate course in Chemical Sciences

PhD thesis

Cycle XXScientific-sector CHIM/06

PhD Candidate:Dr. Melissa Paoletti

Tutors:Prof. Enrico MarcantoniDr. Gianluca Paniccià

Page 2: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Lewis acids in the preparation of the

heterocyclic compounds: synthesis and

characterization of the impurities of API

PhD thesis – Cycle XX

17 March 2008

Page 3: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Characterization of Reference Standards

Identification of unknown impurities

Collaboration with Collaboration with Pfizer,Pfizer,

Ascoli Piceno PlantAscoli Piceno Plant

- Analysis

- Synthesis New methodologies for the synthesis of compounds of pharmaceutical interest

Synthesis of impurities

PhD thesis – Cycle XX

17 March 2008

Page 4: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Lewis acidsLewis acids

TiCl4

Synthesis of β-hydroxy esters

CeCl3•7H2O – NaI

- Knoevenagel condensation- Azides transformation to Primary Amines

CeCl3•7H2O/NaI on SiO2

- Garcia Gonzàlez reaction- Friedel-Crafts reaction

Page 5: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Titanium CompoundsTitanium Compounds

TiX4 derivates are the most commonly used and X anions largely influence the strength of the acid; in fact, if X is an alkoxy group the Lewis acid is a weak while with halogens or triflates its strength increases dramatically.

TiCl4

oxyphilic character

favourite octahedral structure

ability to chelate

Page 6: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Diastereoselective synthesis of tertiary Diastereoselective synthesis of tertiary alcohols by nucleophilic addition to α–alcohols by nucleophilic addition to α–

substituted-β-keto esterssubstituted-β-keto esters

PhD thesis – Cycle XX

17 March 2008

The synthetic strategy adopted for the stereoselective addition of RMgX-CeCl3 species to β-keto amides was based on their conversion into the corresponding titanium cyclic titanium cyclic complexes. complexes.

R OR1

O O

TiCl4

R2MgX-CeCl3R OR1

OHO

R2

Marcantoni, E., Massaccesi, M., Paoletti, M., Sambri, L.; Arkivok, 2006, 49-58

Page 7: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Diastereoselective synthesis of tertiary Diastereoselective synthesis of tertiary alcohols by nucleophilic addition to α–alcohols by nucleophilic addition to α–

substituted-β-keto esterssubstituted-β-keto esters

PhD thesis – Cycle XX

17 March 2008

R OR1

O O

TiCl4

R2MgX-CeCl3; -78°CR OR1

OHO

R2

Marcantoni, E., Massaccesi, M., Paoletti, M., Sambri, L.; Arkivok, 2006, 49-58

Page 8: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Diastereoselective synthesis of tertiary Diastereoselective synthesis of tertiary alcohols by nucleophilic addition to α–alcohols by nucleophilic addition to α–

substituted-β-keto esterssubstituted-β-keto esters

PhD thesis – Cycle XX

17 March 2008

• High diastereoselectivity• moderate-to-good efficiency

Marcantoni, E., Massaccesi, M., Paoletti, M., Sambri, L.; Arkivok, 2006, 49-58

Page 9: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Diastereoselective synthesis of tertiary Diastereoselective synthesis of tertiary alcohols by nucleophilic addition to α–alcohols by nucleophilic addition to α–

substituted-β-keto esterssubstituted-β-keto esters

PhD thesis – Cycle XX

17 March 2008

The nature of the carbonyl-substituent in the β-keto ester substrate.

Marcantoni, E., Massaccesi, M., Paoletti, M., Sambri, L.; Arkivok, 2006, 49-58

Page 10: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Ce

FRIENDLY LEWIS ACIDFRIENDLY LEWIS ACID

Discovered in 1803 by Berzelius and Hisinger

Lanthanide

Oxidation state III and IV

CeCl3

High stability towards water

Low Toxicity

Cerium saltsCerium saltsPhD thesis – Cycle XX

17 March 2008

Ready availability at low cost

CeCl3.7H2O

Page 11: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

CeClCeCl337H7H22O-NaIO-NaI

Solvent-freeconditions

Formation of new bonds

Solidsupport

Chemo- and regioselectivity

“Friendly” Lewis acid

CeCl3·7H2ONaI

Page 12: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.; Beleggia, R.; Giuli, S., Giuliani, A., Marcantoni, E.; Massaccesi, M., Paoletti, M., Tetrahedron Letters, 2006, 47, 6501-6504.

The CeClThe CeCl33..7H7H22O-NaI system as promoter in O-NaI system as promoter in

the synthesis of functionalized the synthesis of functionalized trisubstituted alkenes viatrisubstituted alkenes via

Knoevenagel condensationKnoevenagel condensationCeCl3

.7H2O-NaI system promotes the addition of CH-acidic compounds to different electrophiles.

R1 H

O EWG1

EWG2

R1 EWG1

EWG2

+cat.

1 2 3

Building blocks useful for the synthesis of natural and non-natural bioactive compounds

• Increased the potentialities of CeCl3.7H2O-

NaI system• major restriction to the broad application of the Knoevenagel reaction

Page 13: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.; Beleggia, R.; Giuli, S., Giuliani, A., Marcantoni, E.; Massaccesi, M., Paoletti, M., Tetrahedron Letters, 2006, 47, 6501-6504.

The CeClThe CeCl33..7H7H22O-NaI system as promoter in O-NaI system as promoter in

the synthesis of functionalized the synthesis of functionalized trisubstituted alkenes viatrisubstituted alkenes via

Knoevenagel condensationKnoevenagel condensation

ArCO2Et

CO2But

6a-fAr H

O CO2Et

CO2But+

4a-f 5

ArCO2Et

COOH

7a-f

CeCl3.7H2O

NaI

CH3CN, r.t.

Reflux

• 1:1.2 ratio between 4a and 5 in a ca. 0.1 M solution in acetonitrile• 1.35 equiv of CeCl3

.7H2O • 1.35 equiv of NaI

Page 14: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.; Beleggia, R.; Giuli, S., Giuliani, A., Marcantoni, E.; Massaccesi, M., Paoletti, M., Tetrahedron Letters, 2006, 47, 6501-6504.

Knoevenagel condensationKnoevenagel condensationEntry Time/h Productb Yield (%)c

1

2

3

4

5

6

5480

40

37

62

64

42

95

97

90

85

91

4a

4f

4b

4c

4d

4e

7a

Aldehydea

CHO

CHO

F3C

CHO

O2N

CHO

H3C

CHO

H3CO

N

CHO

2.5

1.5

0.5

3.5

4.0

1.5

r.t.

r.t.

r.t.

r.t.

r.t.

r.t.

reflux

reflux

reflux

reflux

reflux

reflux

CO2Et

COOH

7b

CO2Et

COOHF3C

7c

CO2Et

COOHO2N

7d

CO2Et

COOHH3C

7e

CO2Et

COOHH3CO

7f

N

CO2Et

COOH

E : Zd

77:23

90:10

93:07

75:25

80:20

60:40

Conditions

• malonate mono acid 7 as unique product isolated • no evidence of ,-unsaturated malonic acids.

fairly stereoselective affording E-isomers in high yields

Page 15: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G., Di Antonio, G., Giovannini, R., Giuli, S., Lanari, S., Paoletti, M., Marcantoni, E., J. Org. Chem. 2008, 73, 1919-1924.

Microwave-Assisted Azides Microwave-Assisted Azides Trasformation to Primary Amines Trasformation to Primary Amines Using Mild and Easily Accessible Using Mild and Easily Accessible

CeClCeCl33..7H7H22O/NaI SystemO/NaI System

CeCl3.7H2O (1.5 eq)

CH3CNR N3

NaI (9 eq)

reflux or MW

R NH2

Page 16: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G., Di Antonio, G., Giovannini, R., Giuli, S., Lanari, S., Paoletti, M., Marcantoni, E., J. Org. Chem. 2008, 73, 1919-1924.

Microwave-Assisted Azides Trasformation to Microwave-Assisted Azides Trasformation to Primary Amines Using Mild and Easily Primary Amines Using Mild and Easily

Accessible CeClAccessible CeCl33..7H7H22O/NaI SystemO/NaI System

CeCl3.7H2O (1.5 eq)

SiO2

R N3

NaI (1.5 eq)

r.t. or reflux

R NH2

CeCl3.7H2O (1.5 eq)

CH3CNR N3

NaI (9 eq)

reflux; 24h

R NH2

(1 eq)

Page 17: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Microwave-Assisted Azides Trasformation to Microwave-Assisted Azides Trasformation to Primary Amines Using Mild and Easily Primary Amines Using Mild and Easily

Accessible CeClAccessible CeCl33..7H7H22O/NaI SystemO/NaI System

Entry Product Yield (%)

1

2

3

75

Starting Material

O2N

N3

O2N

NH2

4

75N3 NH2

75

N3 NH2

90N3 NH2H3CO H3CO

O O

Bartoli, G., Di Antonio, G., Giovannini, R., Giuli, S., Lanari, S., Paoletti, M., Marcantoni, E., J. Org. Chem. 2008, 73, 1919-1924.

Page 18: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Azides Trasformation to Primary AminesAzides Trasformation to Primary Amines

Bartoli, G., Di Antonio, G., Giovannini, R., Giuli, S., Lanari, S., Paoletti, M., Marcantoni, E., J. Org. Chem 2008, 73, 1919-1924.

N3 NH2

CeCl3.7H2O

solvent, MW

NaI

Entry NaI CeCl3.7H2O Conditions/Time

(min)Temp.(°C) Yields (%)

1 1.00 eq 1.50 eq 5W; EtOH / 30 90 31

2 2.00 eq 1.50 eq 5W; EtOH / 30 70 20

3 2.00 eq 1.50 eq 40W; EtOH / 30 90 35

4 9.00 eq 1.50 eq 40W; EtOH / 30 100 36

5 9.00 eq 1.50 eq 40W; H2O / 60 100 0

6 2.00 eq 1.50 eq 40W; CH3CN / 30 100 38

7 9.00 eq 1.50 eq 10W; CH3CN / 20 100 86

• Diminution of the reaction time• Higher yields

Page 19: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

GarciaGarcia GonzàlezGonzàlez reaction reaction [2][2]

O

OH

HOHO

OH OH

O O

+

90°C, Reflux

ZnCl2, EtOH

O

O

HO

OH

OH

OH

Starting

material

Glycosidase inhibitors

O

COOEt

HO

OH

HO

HO

PhD thesis – Cycle XX

17 March 2008

[2] F. Garcia Gonzàles, Adv. Carbohydr. Chem. 1956, 11, 97

O

O

X

RHO

OHLipophilicity

ChiralityFlexibility

HydrophilicityRigidity

n

Page 20: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

O

OH

HOHO

OH OH

O O

O+

O

T=90°C, 5h

CeCl3 7 H2O, H2OO

OHHO

(93%)

6 87

Sugar Time (h) Product1,3-dione

D-GlusoseOEt

O O

O

OOEt

O

OHHO

8 82D-GalactoseOEt

O O

O

OOEt

O

OHHO

7 90D-Arabinose

O O

O

O

HO

HO

OH

Yield(%)

PhD thesis – Cycle XX

17 March 2008

Garcia Gonzàlez Garcia Gonzàlez reaction reaction [3][3]

[3] A.K. Misra, G. Aghihotri Carbohydrate Research 2004, 339, 1381

Page 21: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

O

OH

HOHO

OH OHOEt

O O

O+

OOEt

CH3CN, 60°C, 1,5h

1 eq CeCl3. 7H2O

0,1 eq NaI

HO

OH

HO

OH

Entry D-GlucoseEthyl

acetoacetateCeCl3

.7H2O NaITime

(h)Temperature

(°C)Yield(%)

1 1 eq 1 eq 0,1 eq - 1,5 60 -

2 1 eq 1 eq 1 eq - 1,5 60 18,5

3 1 eq 1,2 eq 1 eq 0,1 eq 1,5 60 54

Garcia Gonzàlez Garcia Gonzàlez reactionreaction

PhD thesis – Cycle XX

17 March 2008

Page 22: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

• Solvent-free

• 0,3 eq of promoter system

• 0,5 g SiO2/mmol D-glucose

2429

40

53

80

95

7570

0

1020

3040

50

6070

8090

100

0,05 0,12 0,25 0,35 0,45 0,5 0,55 0,65

grams of Silica gel for 1 mmol of D-Glucose

yiel

d %

HP

LC

of

5aa

O

O

HO

OH

OH

OH

O

OH

HOHO

OH OH

O O

+

SiO2 T=50°C

CeCl3 7 H2O - NaI

Garcia Gonzàlez reaction Garcia Gonzàlez reaction solvent-freesolvent-free

PhD thesis – Cycle XX

36 85

Sugar Time (h) Yield(%)1,3-dione

O OD-Glusose

Temperature (°C)

50

D-Mannose

O O36 8850

D-Galactose

O O48 8550

17 March 2008

Bartoli, G.; Fernàndez-Bolanõs, J.G.; Di Antonio, G.; Foglia, G.; Giuli S.; Gunnella, R.; Mancinelli, M.; Marcantoni, E.; Paoletti, M. J. Org. Chem. 2007, 72, 6029-6036.

Page 23: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

The solid supportSiO2

NaI is essential for the reaction

PhD thesis – Cycle XX

17 March 2008

CeClCeCl33•7H•7H22O-NaI-SiOO-NaI-SiO22

• gives a better yield of product

• facilitates the work up of the reaction mixture • permits the reaction to be accomplished without solvent

Bartoli, G.; Fernàndez-Bolanõs, J.G.; Di Antonio, G.; Foglia, G.; Giuli S.; Gunnella, R.; Mancinelli, M.; Marcantoni, E.; Paoletti, M. J. Org. Chem. 2007, 72, 6029-6036.

H2O is essential for the reaction

Page 24: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.; Di Antonio, G.; Giuli, S.; Marcantoni, E.; Marcolini, M.; Paoletti, M., Synthesis, 2008, 2, 320-324.

The CeClThe CeCl33..7H7H22O-NaI-SiOO-NaI-SiO22 as efficient as efficient

promoter for Friedel-Crafts reaction of promoter for Friedel-Crafts reaction of Indoles to Nitroalkenes in solvent-free Indoles to Nitroalkenes in solvent-free

conditionsconditions

NH

NH

CeCl3.7H2O

NaI, SiO2

+R

NO2

X XR

NO2

Page 25: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.;Di Antonio, G.; Giuli, S.; Marcantoni, E.; Marcolini, M.; Paoletti, M., Synthesis, 2008, 2, 320-324.

Friedel-Crafts reaction of Indoles to Friedel-Crafts reaction of Indoles to NitroalkenesNitroalkenes

NH

NH

CeCl3.7H2O

NaI, SiO2

+Ph

NO2

X XPh

NO2

Entry Time (h) Yield(%)

1

Product

4

3

2

NH

Indole

NH

Ph

NO2

NH

Ph

NO2

H3CO

NH

Ph

NO2

NC

NH

NH

NH

NH

Ph

NO2

HO

8

4

18

24

96

92

85

74

H3CO

NC

HO

• 0.3 eq CeCl3.7H2O

• 0.3 equiv of NaI • SiO2 (0.5 g/mmol of nitroalkene)• solvent-free conditions

Page 26: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.;Di Antonio, G.; Giuli, S.; Marcantoni, E.; Marcolini, M.; Paoletti, M., Synthesis, 2008, 2, 320-324.

NH

NH

CeCl3.7H2ONaI, SiO2

1a 2b

+

3ab

N NO2

Boc

NBoc

NO2

H

r.t., 2h, 89%

N

NCH3

CH3

NH7

3-(2-nitroethyl)indolyl derivative

The CeClThe CeCl33..7H7H22O-NaI-SiOO-NaI-SiO22 as efficient promoter for as efficient promoter for

Friedel-Crafts reaction of Indoles to Nitroalkenes Friedel-Crafts reaction of Indoles to Nitroalkenes in solvent-free conditionsin solvent-free conditions

-carboline ring of the (-)-(S)-Brevicolline

Carex Brevicollis

Page 27: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Bartoli, G.;Di Antonio, G.; Giuli, S.; Marcantoni, E.; Marcolini, M.; Paoletti, M., Synthesis, 2008, 2, 320-324.

Friedel-Crafts reaction of Indoles to Friedel-Crafts reaction of Indoles to NitroalkenesNitroalkenes

NH

NH

R1

CeCl3.7H2O

NaI, SiO21 2

+

3

XR1

H

R2NO2 X NO2

R2

NH

R1

4

X R2

NH2NH5

NH

XR1

R2

R3

NH

6

N

XR1

R2

R3

Reduction

Cyclization

R3CHO

Aromatizationtetrahydro- carboline tryptamine derivative

Page 28: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Synthesis and Synthesis and Chracterization of ImpuritiesChracterization of Impurities

Page 29: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Characterization of Reference Standards

Identification of unknown impurities

Collaboration with Collaboration with Pfizer,Pfizer,

Ascoli Piceno PlantAscoli Piceno Plant

- Analysis

- Synthesis New methodologies for the synthesis of compounds of pharmaceutical interest

Synthesis of impurities

PhD thesis – Cycle XX

18 December 2007

Page 30: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

ImpuritiesImpuritiesIf a material previously considered to be pure can be resolved into more than one component, that material can be redefined into new

terms of purity and impurity.

ORGANIC INORGANIC RESIDUAL SOLVENT

TOXIC ORDINARY

Page 31: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Synthesis of Impurities II and III of Synthesis of Impurities II and III of EtofamideEtofamide

O

NH

OO2N

N-[4-(4-nitrophenoxy)benzyl]-N-(2-ethoxyethyl)amine

O

NO2N

O

NO2

O

N,N-di-[4-(4-nitrophenoxy)benzyl]-N-(2-ethoxyethyl)amine

PhD thesis – Cycle XX

17 March 2008

Page 32: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

18 December 2007

EtofamideEtofamide

O

NO2N

O

Cl

Cl

O

API of Kitnos

Page 33: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Synthesis of EtofamideSynthesis of Etofamide

The tertiary base impurity is the product of the reaction of 4-chloromethyl-4’-nitrodiphenyl ether with N-(2-ethoxyethyl)-N-[4-(4-nitrophenoxy)benzyl]amine intermediate.

PhD thesis – Cycle XX

17 March 2008

Page 34: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

• INTRODUCTION

Chemical name (based on IUPAC rules):N-(2-ethoxyethyl)-N-[4-(4-nitrophenoxy)benzyl] amine.

Chemical Abstract Services (CAS) Registry Number: 101588-13-0.

Molecular Formula: C17H20N2O4.

Structural Formula:

O

NH

OO2N

Impurity II of EtofamideImpurity II of Etofamide

PhD thesis – Cycle XX

17 March 2008

Page 35: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Synthesis of Impurity II of EtofamideSynthesis of Impurity II of Etofamide

PhD thesis – Cycle XX

17 March 2008

O

NH

OO2N

O

O2NCl H2N

O

1

23

Free solvent;r.t.

O

O2N

(CH2O)n; H3PO4

HCl conc; CH3CO2Hrif. 85°C (50h)

4 90%

J. Am. Chem. Soc., 1953, 75, 5877-5880 Il Farmaco- Ed. Sc.-, 1957, XIII, 139-151

Page 36: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Impurity III of EtofamideImpurity III of Etofamide

PhD thesis – Cycle XX

17 March 2008

INTRODUCTION

Chemical name (based on IUPAC rules):N-(2-ethoxyethyl)-N,N-di-[4-(4-nitrophenoxy)benzyl] amine

Molecular Formula: C30H29N3O7

Structural Formula:

O

NO2N

O

NO2

O

Page 37: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Synthesis of Impurity III of Synthesis of Impurity III of EtofamideEtofamide

PhD thesis – Cycle XX

17 March 2008

O

NH

OO2N

O

O2NCl

1

3

Et3N,DMF dry,rif.

O

NO2N

O O

NO2

2

80%

Page 38: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

IsomaltitolIsomaltitol

PhD thesis – Cycle XX

17 March 2008

INTRODUCTION

Chemical name (based on IUPAC rules):(2R, 3S, 4S, 5S)-6-{[( 2R, 3S, 4R, 5R, 6S)- 3,4,5- trihydroxy-6-(hydroxymethyl) terahydro-2H-2 pyranyl] oxy}hexane-1,2,3,4,5- pentaol

Trivial name: 6-O-α-(D)-Glucopyranosyl-D-glucitol.

Chemical Abstract Services (CAS) Registry Number: 534-73-6.

Molecular Formula: C12H24O11

Structural Formula:

O

OH

HO

HO

OOH

OH

OH

OH

OH

OH

Page 39: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Synthesis of IsomaltitolSynthesis of Isomaltitol

PhD thesis – Cycle XX

17 March 2008

O

OH

HO

HO

O

OH

OH

OH

OH

OH

OO

OH

HO

HO

O

OH

OH

OH

OH

OH

OHNaBH4

r.t.; 48h

Thermochimica Acta 1996, 271, 149-153.

Page 40: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

IsomaltIsomalt

PhD thesis – Cycle XX

17 March 2008

Thermochimica Acta 1996, 271, 149-153.

Page 41: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

IsomaltitolIsomaltitol

PhD thesis – Cycle XX

17 March 2008

Commercial Isomaltitol Synthesized Isomaltitol

Page 42: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

RFT METODO 1RFT METODO 1RIDUZIONE COSTI DI APPROVVIGIONAMENTO RIDUZIONE COSTI DI APPROVVIGIONAMENTO

PER ISO-MALTITOLOPER ISO-MALTITOLO

OBIETTIVO:OBIETTIVO: Riduzione costi per l’acquisto del reagente necessario all’analisi Riduzione costi per l’acquisto del reagente necessario all’analisi

PROBLEMA: PROBLEMA: Elevato costo del reagente iso-maltitolo utilizzato nel metodo 6500QW vs 3 per la determinazione delle sostanze correlate del Mannitolo mediante HPLC (Entrata in vigore del nuovo metodo di Pharmacopeia Europea )

MMISURAISURAQUANTITA’ ANNUA NECESSARIA:QUANTITA’ ANNUA NECESSARIA: 5.000 mg per analisi 5.000 mg scorta TOT = 10.000 mg

COSTO REAGENTE:COSTO REAGENTE: 1.340,00 Euro ogni 50mg

COSTO TOTALE: 268.000,00 Euro all’annoCOSTO TOTALE: 268.000,00 Euro all’anno

DDEFINIZIONEEFINIZIONE

CONTROLLOCONTROLLO•SOLUZIONI 1 E 2 APPLICATE IN MODO SINERGICO:

RISPARMIO DI 267.700,00 EURO all’annoRISPARMIO DI 267.700,00 EURO all’anno

______________________________

•SOLUZIONI 3 IN CORSO DI VALUTAZIONE

•SOLUZIONE 4 = NESSUN VANTAGGIO

COSTI

ANALISIANALISI

ALTO COSTO REAGENTE

Materiali Persone Misura

Metodi Macchine Ambiente

Quantità ordine

Costo Reagente

Fornitore (Sigma)Purezza Reagente

Metodo Analitico EP

IIMPLEMENTAZIONEMPLEMENTAZIONE

BE

NE

FIC

I

2. Modifica metodo mediante cambio della pesata (riduzione Pesata)

4. Altro fornitore

1. Sintesi del reagente in esame, per riduzione dell’isomaltoso (600 euro al grammo), effettuata dal gruppo di ricerca del Prof. Marcantoni (Dip.di Scienze Chimiche,Università degli Studi di Camerino, Responsabile Scientifico: Prof. R. Ballini)

3. Stabilità della soluzione di iso-maltitolo

IL TEAM

Page 43: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Cabergoline N-OxideCabergoline N-OxidePhD thesis – Cycle XX

17 March 2007

INTRODUCTION

Chemical name (based on IUPAC rules):(3-{{[(6aR,9R,10aR)-7-Allyl-4,6,6a,7,8,9,10,10a-octahydroindolo[4,3-fg]quinolin-9yl]carbonyl}[(ethylamino)carbonyl]amino}propyl)(dimethyl)ammoniumolate.

Empirical Formula: C26H37N5O2

Structural Formula:

N

N

O N N

CH3

CH3

OHN CH3

H

H

H

O

Page 44: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

CabergolineCabergolinePhD thesis – Cycle XX

17 March 2008

HN

N

O N N

CH3

CH3

OHN CH3

H

H

HN

N

O

H

OH

9,10-dihdrolysergic acid

API of DOSTINEX:•Hyperprolactinemia (dosage: 0.25mg and 0.5mg per tablets)• Anti-Parkinson (dosage: 1, 2 and 4mg per tablets)

Page 45: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PhD thesis – Cycle XX

17 March 2008

Chracterization of Chracterization of ImpuritiesImpurities

Page 46: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PABAPABA

PhD thesis – Cycle XX

17 March 2008

Be-Total HDBe-Total HD sugar-coated tabletssugar-coated tablets

O OH

NH2

p-Aminobenzoic Acid

PABA is an essential nutrient for some bacteria and is considered to be in the B-complex vitamin family (Vitamin Bx).

Page 47: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Impurity of Impurity of PABAPABA

PhD thesis – Cycle XX

17 March 2008

Page 48: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Impurity of Impurity of PABAPABA

PhD thesis – Cycle XX

17 March 2008

Page 49: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

PABAPABA

PhD thesis – Cycle XX

17 March 2008

The intake of PABA and PABA ester is associated with the same efficacy and safety as free PABA alone.

Page 50: Lewis acids in the preparation of the heterocyclic compounds: synthesis and characterization of the impurities of API 2004/05 – 2006/07 SCHOOL OF ADVANCED

Acknowledgements

Colleagues at the laboratory and all the people that have collaborated in the

development of the projects

PhD thesis – Cycle XX

Prof. Enrico Marcantoni Prof. Roberto Ballini Dott.ssa Sandra Giuli

17 March 2008

Dr. Gianluca Paniccià Dr. Orenzo Agostini Sig. Terenzio De Angelis