Abstract
Ethylene remains one of the most valuable chemical feedstocks. Currently the industrial conversion of ethane to ethylene is achieved largely by steam cracking. The catalytic, highly exothermic oxidative dehydrogenation (ODH) of ethane with O2 is a challenging alternative that has been extensively studied on the laboratory scale. Here we investigate the possibility of using disulfur (S2) vapor as a thermodynamically “soft” oxidant for catalytically converting ethane to ethylene (“SODH”). Investigating a series of four catalysts we report a maximum ethylene yield of 76 % over an earth-abundant FeSx-based catalyst (maximum 90.2 % C2H4 selectivity at 820 °C). Yield and selectivity are stable for 50 hours on stream. The SODH rate law is 1st order in ethane and (Formula presented.) order in S2, supporting a proposed Mars van Krevelen-like mechanism at temperatures '700 °C. Furthermore, conversion and selectivity become insensitive to catalyst identity at temperatures '860 °C, suggesting the intrusion of radical pathways.
Original language | English (US) |
---|---|
Pages (from-to) | 4538-4542 |
Number of pages | 5 |
Journal | ChemCatChem |
Volume | 12 |
Issue number | 18 |
DOIs | |
State | Published - Sep 17 2020 |
Funding
We thank the Center for Innovative and Strategic Transformation of Alkane Resources (CISTAR, NSF award number: 1647722) for funding this project. We thank Professor Fabio H. Ribeiro of Purdue U., Dr. Matthias Peter of BASF as well as Professor Justin M. Notestein and Dr. Neil Schweitzer of Northwestern U. for helpful suggestions. We thank the Center for Innovative and Strategic Transformation of Alkane Resources (CISTAR, NSF award number: 1647722) for funding this project. We thank Professor Fabio H. Ribeiro of Purdue U., Dr. Matthias Peter of BASF as well as Professor Justin M. Notestein and Dr. Neil Schweitzer of Northwestern U. for helpful suggestions.
Keywords
- Ethane
- Ethylene
- Heterogeneous Catalysis
- Oxidative Dehydrogenation
- Sulfur
ASJC Scopus subject areas
- Catalysis
- Physical and Theoretical Chemistry
- Organic Chemistry
- Inorganic Chemistry