Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid

The single-pot efficient oxidation of ethane to acetic acid catalysed by Au(I) or Au(III) compounds, chlorotriphenylphosphinegold(I) (<b>1</b>), chlorotrimethylphosphinegold(I) (<b>2</b>), 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidenegold(I) chloride (<b>3</b>)...

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Main Authors: Ana P. C. Ribeiro, Inês A. S. Matias, Sónia A. C. Carabineiro, Luísa M. D. R. S. Martins
Format: Article
Language:English
Published: MDPI AG 2022-01-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/12/2/165
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author Ana P. C. Ribeiro
Inês A. S. Matias
Sónia A. C. Carabineiro
Luísa M. D. R. S. Martins
author_facet Ana P. C. Ribeiro
Inês A. S. Matias
Sónia A. C. Carabineiro
Luísa M. D. R. S. Martins
author_sort Ana P. C. Ribeiro
collection DOAJ
description The single-pot efficient oxidation of ethane to acetic acid catalysed by Au(I) or Au(III) compounds, chlorotriphenylphosphinegold(I) (<b>1</b>), chlorotrimethylphosphinegold(I) (<b>2</b>), 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidenegold(I) chloride (<b>3</b>), dichloro(2-pyridinecarboxylato)gold(III) (<b>4</b>), homogenous and supported on different carbon materials: activated carbon (AC), multi-walled carbon nanotubes (CNT) and carbon xerogel (CX), oxidised with nitric acid followed by treatment with NaOH (-ox-Na), is reported. The reactions were performed in water/acetonitrile. The materials were selective for the production of acetic acid, with no trace of by-products being detected. The best homogenous catalysts were complexes <b>2</b> and <b>3</b> which showed the highest ethane conversion and an acetic acid yield of ca. 21%, followed by <b>4</b> and <b>1</b>. The heterogenised materials showed much better activity than the homogenous counterparts, with acetic acid yields up to 41.4% for <b>4</b>@CNT-ox-Na, and remarkable selectivity (with acetic acid being the only product detected). The heterogenised catalysts with the best results were reused up to five cycles, with no significant loss of activity, and maintaining high selectivity for acetic acid. <b>4</b>@CNT-ox-Na showed not only the best catalytic activity but also the best stability during the recycling runs.
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spelling doaj.art-4bafec3a2def43529f69fddee4edca222023-11-23T19:12:18ZengMDPI AGCatalysts2073-43442022-01-0112216510.3390/catal12020165Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic AcidAna P. C. Ribeiro0Inês A. S. Matias1Sónia A. C. Carabineiro2Luísa M. D. R. S. Martins3Centro de Química Estrutural, Institute of Molecular Sciences, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, PortugalCentro de Química Estrutural, Institute of Molecular Sciences, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, PortugalCentro de Química Estrutural, Institute of Molecular Sciences, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, PortugalCentro de Química Estrutural, Institute of Molecular Sciences, Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, PortugalThe single-pot efficient oxidation of ethane to acetic acid catalysed by Au(I) or Au(III) compounds, chlorotriphenylphosphinegold(I) (<b>1</b>), chlorotrimethylphosphinegold(I) (<b>2</b>), 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidenegold(I) chloride (<b>3</b>), dichloro(2-pyridinecarboxylato)gold(III) (<b>4</b>), homogenous and supported on different carbon materials: activated carbon (AC), multi-walled carbon nanotubes (CNT) and carbon xerogel (CX), oxidised with nitric acid followed by treatment with NaOH (-ox-Na), is reported. The reactions were performed in water/acetonitrile. The materials were selective for the production of acetic acid, with no trace of by-products being detected. The best homogenous catalysts were complexes <b>2</b> and <b>3</b> which showed the highest ethane conversion and an acetic acid yield of ca. 21%, followed by <b>4</b> and <b>1</b>. The heterogenised materials showed much better activity than the homogenous counterparts, with acetic acid yields up to 41.4% for <b>4</b>@CNT-ox-Na, and remarkable selectivity (with acetic acid being the only product detected). The heterogenised catalysts with the best results were reused up to five cycles, with no significant loss of activity, and maintaining high selectivity for acetic acid. <b>4</b>@CNT-ox-Na showed not only the best catalytic activity but also the best stability during the recycling runs.https://www.mdpi.com/2073-4344/12/2/165ethane oxidationacetic acidgoldcarbonheterogeneous catalysis
spellingShingle Ana P. C. Ribeiro
Inês A. S. Matias
Sónia A. C. Carabineiro
Luísa M. D. R. S. Martins
Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
Catalysts
ethane oxidation
acetic acid
gold
carbon
heterogeneous catalysis
title Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
title_full Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
title_fullStr Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
title_full_unstemmed Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
title_short Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
title_sort commercial gold complexes supported on functionalised carbon materials as efficient catalysts for the direct oxidation of ethane to acetic acid
topic ethane oxidation
acetic acid
gold
carbon
heterogeneous catalysis
url https://www.mdpi.com/2073-4344/12/2/165
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AT soniaaccarabineiro commercialgoldcomplexessupportedonfunctionalisedcarbonmaterialsasefficientcatalystsforthedirectoxidationofethanetoaceticacid
AT luisamdrsmartins commercialgoldcomplexessupportedonfunctionalisedcarbonmaterialsasefficientcatalystsforthedirectoxidationofethanetoaceticacid