Silica-supported tantalum hydride, (SiO)2Ta-H (1), proves to be the first single-site catalyst for the direct non-oxidative coupling transformation of methane into ethane and hydrogen at moderate temperatures, with a high selectivity (>98%). The reaction likely involves the tantalum-methyl-methylidene species as a key intermediate, where the methyl ligand can migrate onto the tantalum-methylidene affording the tantalum-ethyl.
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http://dx.doi.org/10.1021/ja800863x | DOI Listing |
ChemSusChem
November 2024
Department of Chemical and Biological Engineering, Tufts University, Medford, Massachusetts, 02155, USA.
Developing improved catalysts for sustainable chemical processes often involves understanding atomistic origins of catalytic activity, selectivity, and stability. Using density functional theory and steady-state kinetic analyses, we probe the elementary steps that form decomposition products that limit selectivity in vinyl acetate (VA) synthesis on Pd surfaces covered with acetate species. Acetate formation and coupling with ethylene control the VA formation catalytic cycle and steady-state coverage, but acetate and ethylene can separately decompose to form CO.
View Article and Find Full Text PDFEES Catal
October 2024
Department of Chemical, Biological, Pharmaceutical and Environmental Sciences and CASPE (INSTM), University of Messina Viale F. Stagno D'Alcontres 31 98166 Messina Italy
[This corrects the article DOI: 10.1039/D4EY00112E.].
View Article and Find Full Text PDFEES Catal
September 2024
Department of Chemical, Biological, Pharmaceutical and Environmental Sciences and CASPE (INSTM), University of Messina, Viale F. Stagno D'Alcontres 31 98166 Messina Italy
The photocatalytic non-oxidative coupling of methane (NOCM) is a highly challenging and sustainable reaction to produce H and C hydrocarbons under ambient conditions using sunlight. However, there is a lack of knowledge, particularly on how to achieve high photocatalytic yield in continuous-flow reactors. To address this, we have developed a novel flow-through photocatalytic reactor for NOCM as an alternative to the conventionally used batch reactors.
View Article and Find Full Text PDFJ Am Chem Soc
August 2024
State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, China.
STAR Protoc
June 2024
Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, Delaware 19716, USA; Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742, USA. Electronic address:
A membrane reactor (MR) offers a solution to overcome thermodynamic equilibrium limitations by enabling in situ product separation, enhancing product yields and energy efficiency. Here we present a protocol for synthesizing a carbon MR that couples a H-permeable carbon molecular sieve hollow fiber membrane and a metal supported on zeolite catalyst for non-oxidative propane and ethane dehydrogenation. We describe steps for catalyst preparation, membrane fabrication, and MR construction.
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