Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes: structure-reactivity relationship

M. Martin-Martinez; A. Álvarez-Montero; L.M. Gómez-Sainero; R.T. Baker; J. Palomar; S. Omar; S. Eser; J.J. Rodriguez

doi:10.1016/j.apcatb.2014.07.017

Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes: structure-reactivity relationship

M. Martin-Martinez, A. Álvarez-Montero, L.M. Gómez-Sainero, R.T. Baker, J. Palomar, S. Omar, S. Eser, J.J. Rodriguez

Research output: Contribution to journal › Article › peer-review

Abstract

This study analyzes the influence of chemical and physical properties of Pd/C and Pt/C hydrodechlorination (HDC) catalysts in the different evolution of their activity during time on stream. Pt/C showed stable activity in the HDC of dichloromethane (DCM) and chloroform (TCM), while Pd/C was deactivated after 90 h of operation, particularly during HDC of DCM. The deactivation of Pd/C catalyst can be attributed to the lower proportion of zero-valent species and larger metal particle size. This appears to hinder the H₂ dissociation, enhance the irreversible chemisorption of reactants and reaction products, and favor coupling reactions (leading to the formation of carbonaceous deposits) and/or metal phase change reactions. The more extensive deactivation of Pd/C in the HDC of DCM is attributed to the stronger chemisorption of the reactant on the catalyst, which leads to the formation of a new PdC_x phase by the incorporation of carbon atoms into the metal lattice.

Original language	English
Pages (from-to)	532-543
Number of pages	12
Journal	Applied Catalysis B: Environmental
Volume	162
Early online date	21 Jul 2014
DOIs	https://doi.org/10.1016/j.apcatb.2014.07.017
Publication status	Published - Jan 2015

Keywords

Hydrodechlorination
Chloromethanes
Deactivation
Pd/C
Pt/C

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10.1016/j.apcatb.2014.07.017

Baker_2014_ACBE_DeactivationAM
Copyright © 2014 Elsevier B.V. NOTICE: this is the author’s version of a work that was accepted for publication in Applied Catalysis B: Environmental. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Applied Catalysis B: Environmental, 162 (2015), DOI: 10.1016/j.apcatb.2014.07.017.
Accepted author manuscript, 2.08 MB

Richard Baker
- rtb5st-andrews.acuk
- School of Chemistry - Senior Lecturer
- Centre for Energy Ethics
- EaSTCHEM
Person: Academic

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Martin-Martinez, M., Álvarez-Montero, A., Gómez-Sainero, L. M., Baker, R. T., Palomar, J., Omar, S., Eser, S., & Rodriguez, J. J. (2015). Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes: structure-reactivity relationship. Applied Catalysis B: Environmental, 162, 532-543. https://doi.org/10.1016/j.apcatb.2014.07.017

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title = "Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes: structure-reactivity relationship",

abstract = "This study analyzes the influence of chemical and physical properties of Pd/C and Pt/C hydrodechlorination (HDC) catalysts in the different evolution of their activity during time on stream. Pt/C showed stable activity in the HDC of dichloromethane (DCM) and chloroform (TCM), while Pd/C was deactivated after 90 h of operation, particularly during HDC of DCM. The deactivation of Pd/C catalyst can be attributed to the lower proportion of zero-valent species and larger metal particle size. This appears to hinder the H2 dissociation, enhance the irreversible chemisorption of reactants and reaction products, and favor coupling reactions (leading to the formation of carbonaceous deposits) and/or metal phase change reactions. The more extensive deactivation of Pd/C in the HDC of DCM is attributed to the stronger chemisorption of the reactant on the catalyst, which leads to the formation of a new PdCx phase by the incorporation of carbon atoms into the metal lattice.",

keywords = "Hydrodechlorination, Chloromethanes, Deactivation, Pd/C, Pt/C",

author = "M. Martin-Martinez and A. {\'A}lvarez-Montero and L.M. G{\'o}mez-Sainero and R.T. Baker and J. Palomar and S. Omar and S. Eser and J.J. Rodriguez",

note = "The authors acknowledge financial support from the Spanish Ministerio de Econom{\'i}a y Competitividad (MINECO) through the project CTM2011-28352. M. Mart{\'i}n Mart{\'i}nez acknowledges the Spanish Ministerio de Ciencia e Innovaci{\'o}n (MICINN) and the European Social Fund (ESF) for her research grant.",

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doi = "10.1016/j.apcatb.2014.07.017",

language = "English",

volume = "162",

pages = "532--543",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

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TY - JOUR

T1 - Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes

T2 - structure-reactivity relationship

AU - Martin-Martinez, M.

AU - Álvarez-Montero, A.

AU - Gómez-Sainero, L.M.

AU - Baker, R.T.

AU - Palomar, J.

AU - Omar, S.

AU - Eser, S.

AU - Rodriguez, J.J.

N1 - The authors acknowledge financial support from the Spanish Ministerio de Economía y Competitividad (MINECO) through the project CTM2011-28352. M. Martín Martínez acknowledges the Spanish Ministerio de Ciencia e Innovación (MICINN) and the European Social Fund (ESF) for her research grant.

PY - 2015/1

Y1 - 2015/1

N2 - This study analyzes the influence of chemical and physical properties of Pd/C and Pt/C hydrodechlorination (HDC) catalysts in the different evolution of their activity during time on stream. Pt/C showed stable activity in the HDC of dichloromethane (DCM) and chloroform (TCM), while Pd/C was deactivated after 90 h of operation, particularly during HDC of DCM. The deactivation of Pd/C catalyst can be attributed to the lower proportion of zero-valent species and larger metal particle size. This appears to hinder the H2 dissociation, enhance the irreversible chemisorption of reactants and reaction products, and favor coupling reactions (leading to the formation of carbonaceous deposits) and/or metal phase change reactions. The more extensive deactivation of Pd/C in the HDC of DCM is attributed to the stronger chemisorption of the reactant on the catalyst, which leads to the formation of a new PdCx phase by the incorporation of carbon atoms into the metal lattice.

AB - This study analyzes the influence of chemical and physical properties of Pd/C and Pt/C hydrodechlorination (HDC) catalysts in the different evolution of their activity during time on stream. Pt/C showed stable activity in the HDC of dichloromethane (DCM) and chloroform (TCM), while Pd/C was deactivated after 90 h of operation, particularly during HDC of DCM. The deactivation of Pd/C catalyst can be attributed to the lower proportion of zero-valent species and larger metal particle size. This appears to hinder the H2 dissociation, enhance the irreversible chemisorption of reactants and reaction products, and favor coupling reactions (leading to the formation of carbonaceous deposits) and/or metal phase change reactions. The more extensive deactivation of Pd/C in the HDC of DCM is attributed to the stronger chemisorption of the reactant on the catalyst, which leads to the formation of a new PdCx phase by the incorporation of carbon atoms into the metal lattice.

KW - Hydrodechlorination

KW - Chloromethanes

KW - Deactivation

KW - Pd/C

KW - Pt/C

U2 - 10.1016/j.apcatb.2014.07.017

DO - 10.1016/j.apcatb.2014.07.017

M3 - Article

AN - SCOPUS:84905370198

SN - 0926-3373

VL - 162

SP - 532

EP - 543

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

ER -

Deactivation behavior of Pd/C and Pt/C catalysts in the gas-phase hydrodechlorination of chloromethanes: structure-reactivity relationship

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Keywords

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