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Issue 20, 2020
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Oxidative dehydrogenation of propane over transition metal sulfides using sulfur as an alternative oxidant

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Abstract

The use of alternative oxidants for the oxidative dehydrogenation of propane (ODHP) is a promising strategy to suppress the facile overoxidation to COx that occurs with O2. Gaseous disulfur (S2) represents a thermodynamically “softer” oxidant that has been underexplored and yet offers a potential route to more selective propylene formation. Here we describe a system for sulfur-ODHP (SODHP). We demonstrate that various metal sulfide catalysts generate unique reaction product distributions, and that propylene selectivities as high as 86% can be achieved at 450–550 °C. For a group of 6 metal sulfide catalysts, apparent activation energies for propylene formation range from 72–134 kJ mol−1 and parallel the corresponding catalyst XPS sulfur binding energies, indicating that M–S bond strength plays a key role in SODHP activity. Kinetic data over a sulfided ZrO2 catalyst indicate a rate law which is first-order in propane and zero-order in sulfur, suggesting that SODHP may occur via a mechanism analogous to the Mars van Krevelen cycle of traditional ODHP. The present results should motivate further studies of SODHP as a route to the selective and efficient oxidative production of propylene.

Graphical abstract: Oxidative dehydrogenation of propane over transition metal sulfides using sulfur as an alternative oxidant

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Article information


Submitted
20 May 2020
Accepted
30 Aug 2020
First published
31 Aug 2020

Catal. Sci. Technol., 2020,10, 6840-6848
Article type
Paper

Oxidative dehydrogenation of propane over transition metal sulfides using sulfur as an alternative oxidant

A. M. Arinaga, S. Liu and T. J. Marks, Catal. Sci. Technol., 2020, 10, 6840
DOI: 10.1039/D0CY01039A

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