期刊
JOURNAL OF CATALYSIS
卷 325, 期 -, 页码 1-8出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2015.02.004
关键词
Carbonylation; Heteropolyacid; Ethanol; Iodide; Rhodium
资金
- Dow Chemical Company
- E.I. DuPont de Nemours Co.
- Northwestern University
- U.S. DOE [DE-AC02-06CH11357]
- NASA Ames Research Center [NNA06CB93G]
- NSF [DMR-0521267]
- Department of Energy [DE-FG02-03ER15457]
- MRSEC program of the National Science Foundation at the Materials Research Center of Northwestern University [DMR-1121262]
- NSEC [NSF EEC-0647560]
- MRSEC [NSF DMR-1121262]
- Keck Foundation
- State of Illinois
Ethanol carbonylation is a potential route to valuable C3 products. Here, Rh supported on porous, Cs-exchanged heteropolyacid Cs3PW12O40, is demonstrated as an effective catalyst for vapor-phase ethanol carbonylation, with higher selectivity and conversion to propionates than existing catalysts. Residual acidity or a Mo polyatom was strongly detrimental to yields. Propionate selectivity was maximized at 96% at 170 degrees C and with added H2O. The catalyst displayed stable selectivity over 30 h on stream and up to 77% conversion. Ethyl iodide is a required co-catalyst but at levels as low as 2% relative to ethanol. XPS and in situ XANES indicate partial Rh reduction, consistent with the formation of low-valent reactive intermediates and slow deactivation through formation of Rh nanoparticles. With further optimization and understanding, these Rh/heteropolyacid catalysts may lead to stable and selective catalysts for the production of propionates through ethanol carbonylation. (C) 2015 Elsevier Inc. All rights reserved.
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