Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 152, Issue 4, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.5135920
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Funding
- U.S. National Science Foundation [CBET-1604605]
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MoO3/gamma-Al2O3 catalysts containing 0.3-3 monolayer (ML) equivalents of MoO3 were prepared, characterized, and tested for ethane oxidative dehydrogenation (ODH) in cyclic redox and co-feed modes. Submonolayer catalysts contain highly dispersed (2D) polymolybdate structures; a complete monolayer and bulk Al-2(MoO4)(3) are present at >1ML loadings. High ethylene selectivity (>90%) in chemical looping (CL) ODH correlates with Mo+VI to Mo+V reduction; COx selectivity is <10% under these conditions. Mo+V and Mo+IV species trigger CH4 production resulting in much higher conversion albeit with <20% selectivity. In CL-ODH, submonolayer catalysts exhibit ethylene selectivities that decrease linearly from 96% at near-zero conversion to 70% at 45% conversion. >1ML catalysts provide higher conversions albeit with 10%-18% lower selectivity and greater selectivity loss with increasing conversion. In co-feed mode, ethylene selectivity drops to <50% at 46% conversion for a 0.6ML catalyst, but selectivity is virtually unaltered for a 3ML catalyst. We infer that at <1ML loadings, small domain size and strong Mo-O-Al bonds decrease 2D polymolybdate reducibility and enhance ethylene selectivity in CL-ODH.
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