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

Allison M. Arinaga, Shanfu Liu, Tobin J. Marks

Research output: Contribution to journalArticlepeer-review

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. This journal is

Original languageEnglish
Pages (from-to)6840-6848
Number of pages9
JournalCatalysis Science and Technology
Volume10
Issue number20
DOIs
Publication statusPublished - Oct 21 2020

ASJC Scopus subject areas

  • Catalysis

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