Efficient Hydrogenolysis of Alkanes at Low Temperature and Pressure Using Tantalum Hydride on MCM-41, and a Quantum Chemical Study

Vivek Polshettiwar; Farhan Ahmad Pasha; Aimery De Mallmann; Sébastien Norsic; Jean Thivolle-Cazat; Jean-Marie Basset

doi:10.1002/cctc.201100130

Efficient Hydrogenolysis of Alkanes at Low Temperature and Pressure Using Tantalum Hydride on MCM-41, and a Quantum Chemical Study

Vivek Polshettiwar, Farhan Ahmad Pasha, Aimery De Mallmann, Sébastien Norsic, Jean Thivolle-Cazat, Jean-Marie Basset

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

15 Scopus citations

Abstract

Hydrogenolysis of hydrocarbons is of considerable technological importance for applications such as the hydroprocessing of petrochemical feedstocks to generate high-value and useful chemicals and fuels. We studied the catalytic activity of tantalum hydride supported on MCM-41 for the hydrogenolysis of alkanes at low temperature and low atmospheric pressure in a dynamic reactor. The reactions proceed with good turnover numbers, and the catalyst could be reused for several times, which makes the overall catalytic process sustainable. We derived the plausible mechanism by using DFT calculations and identified the preferred pathways by the analysis of potential energy surface. Our results and the proposed reaction mechanism demonstrate the viability of the "catalyst-by-design" approach. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Original language	English (US)
Pages (from-to)	363-369
Number of pages	7
Journal	ChemCatChem
Volume	4
Issue number	3
DOIs	https://doi.org/10.1002/cctc.201100130
State	Published - Feb 10 2012

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The authors thank ESCPE-Lyon, CNRS, and KAUST for financial and logistical support.

ASJC Scopus subject areas

Inorganic Chemistry
Physical and Theoretical Chemistry
Organic Chemistry
Catalysis

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title = "Efficient Hydrogenolysis of Alkanes at Low Temperature and Pressure Using Tantalum Hydride on MCM-41, and a Quantum Chemical Study",

abstract = "Hydrogenolysis of hydrocarbons is of considerable technological importance for applications such as the hydroprocessing of petrochemical feedstocks to generate high-value and useful chemicals and fuels. We studied the catalytic activity of tantalum hydride supported on MCM-41 for the hydrogenolysis of alkanes at low temperature and low atmospheric pressure in a dynamic reactor. The reactions proceed with good turnover numbers, and the catalyst could be reused for several times, which makes the overall catalytic process sustainable. We derived the plausible mechanism by using DFT calculations and identified the preferred pathways by the analysis of potential energy surface. Our results and the proposed reaction mechanism demonstrate the viability of the {"}catalyst-by-design{"} approach. {\textcopyright} 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.",

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AU - Polshettiwar, Vivek

AU - Pasha, Farhan Ahmad

AU - De Mallmann, Aimery

AU - Norsic, Sébastien

AU - Thivolle-Cazat, Jean

AU - Basset, Jean-Marie

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: The authors thank ESCPE-Lyon, CNRS, and KAUST for financial and logistical support.

PY - 2012/2/10

Y1 - 2012/2/10

N2 - Hydrogenolysis of hydrocarbons is of considerable technological importance for applications such as the hydroprocessing of petrochemical feedstocks to generate high-value and useful chemicals and fuels. We studied the catalytic activity of tantalum hydride supported on MCM-41 for the hydrogenolysis of alkanes at low temperature and low atmospheric pressure in a dynamic reactor. The reactions proceed with good turnover numbers, and the catalyst could be reused for several times, which makes the overall catalytic process sustainable. We derived the plausible mechanism by using DFT calculations and identified the preferred pathways by the analysis of potential energy surface. Our results and the proposed reaction mechanism demonstrate the viability of the "catalyst-by-design" approach. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

AB - Hydrogenolysis of hydrocarbons is of considerable technological importance for applications such as the hydroprocessing of petrochemical feedstocks to generate high-value and useful chemicals and fuels. We studied the catalytic activity of tantalum hydride supported on MCM-41 for the hydrogenolysis of alkanes at low temperature and low atmospheric pressure in a dynamic reactor. The reactions proceed with good turnover numbers, and the catalyst could be reused for several times, which makes the overall catalytic process sustainable. We derived the plausible mechanism by using DFT calculations and identified the preferred pathways by the analysis of potential energy surface. Our results and the proposed reaction mechanism demonstrate the viability of the "catalyst-by-design" approach. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

UR - http://hdl.handle.net/10754/562094

UR - http://doi.wiley.com/10.1002/cctc.201100130

UR - http://www.scopus.com/inward/record.url?scp=84857525790&partnerID=8YFLogxK

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DO - 10.1002/cctc.201100130

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JF - ChemCatChem

IS - 3

ER -

Efficient Hydrogenolysis of Alkanes at Low Temperature and Pressure Using Tantalum Hydride on MCM-41, and a Quantum Chemical Study

Abstract

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ASJC Scopus subject areas

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