Bent Carbon Surface Moieties as Active Sites on Carbon Catalysts for Phosgene Synthesis

Navneet K. Gupta; Anastasia Pashigreva; Evgeny A. Pidko; Emiel J.M. Hensen; Leslaw Mleczko; Stefan Roggan; Erika E. Ember; Johannes A. Lercher

doi:10.1002/anie.201508922

Bent Carbon Surface Moieties as Active Sites on Carbon Catalysts for Phosgene Synthesis

Navneet K. Gupta, Anastasia Pashigreva, Evgeny A. Pidko, Emiel J.M. Hensen, Leslaw Mleczko, Stefan Roggan, Erika E. Ember, Johannes A. Lercher

Chair of Chemical Technology II

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

28 Scopus citations

Abstract

Active sites in carbon-catalyzed phosgene synthesis from gaseous CO and Cl₂ have been identified using C₆₀ fullerene as a model catalyst. The carbon atoms distorted from sp² coordination in non-planar carbon units are concluded to generate active Cl₂. Experiments and density functional theory calculations indicate the formation of a surface-bound [C₆₀⋯Cl₂] chlorine species with radical character as key intermediate during phosgene formation. It reacts rapidly with physisorbed CO in a two-step Eley-Rideal-type mechanism.

Original language	English
Pages (from-to)	1728-1732
Number of pages	5
Journal	Angewandte Chemie International Edition in English
Volume	55
Issue number	5
DOIs	https://doi.org/10.1002/anie.201508922
State	Published - 26 Jan 2016

Keywords

chlorine
density functional calculations
fullerenes
phosgene
reaction mechanisms

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abstract = "Active sites in carbon-catalyzed phosgene synthesis from gaseous CO and Cl2 have been identified using C60 fullerene as a model catalyst. The carbon atoms distorted from sp2 coordination in non-planar carbon units are concluded to generate active Cl2. Experiments and density functional theory calculations indicate the formation of a surface-bound [C60⋯Cl2] chlorine species with radical character as key intermediate during phosgene formation. It reacts rapidly with physisorbed CO in a two-step Eley-Rideal-type mechanism.",

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AU - Gupta, Navneet K.

AU - Pashigreva, Anastasia

AU - Pidko, Evgeny A.

AU - Hensen, Emiel J.M.

AU - Mleczko, Leslaw

AU - Roggan, Stefan

AU - Ember, Erika E.

AU - Lercher, Johannes A.

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N2 - Active sites in carbon-catalyzed phosgene synthesis from gaseous CO and Cl2 have been identified using C60 fullerene as a model catalyst. The carbon atoms distorted from sp2 coordination in non-planar carbon units are concluded to generate active Cl2. Experiments and density functional theory calculations indicate the formation of a surface-bound [C60⋯Cl2] chlorine species with radical character as key intermediate during phosgene formation. It reacts rapidly with physisorbed CO in a two-step Eley-Rideal-type mechanism.

AB - Active sites in carbon-catalyzed phosgene synthesis from gaseous CO and Cl2 have been identified using C60 fullerene as a model catalyst. The carbon atoms distorted from sp2 coordination in non-planar carbon units are concluded to generate active Cl2. Experiments and density functional theory calculations indicate the formation of a surface-bound [C60⋯Cl2] chlorine species with radical character as key intermediate during phosgene formation. It reacts rapidly with physisorbed CO in a two-step Eley-Rideal-type mechanism.

KW - chlorine

KW - density functional calculations

KW - fullerenes

KW - phosgene

KW - reaction mechanisms

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Bent Carbon Surface Moieties as Active Sites on Carbon Catalysts for Phosgene Synthesis

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