Journal
JOURNAL OF CATALYSIS
Volume 343, Issue -, Pages 86-96Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2016.03.016
Keywords
CO2 hydrogenation; Methanation; Reverse water gas shift; DFT; Microkinetic model; Selectivity
Categories
Funding
- University of California, Riverside
- National Science Foundation Grant [CHE-1301019]
- National Science Foundation [OCI-1053575]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1301019] Funding Source: National Science Foundation
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The mechanism of CO2 reduction by H-2 at atmospheric pressure was investigated on Ru(0001) by coupling density functional theory (DFT) calculations with mean-field microkinetic modeling. The initial CO2 hydrogenation step leading to CH4 production was shown to occur through CO2 dissociation and subsequent hydrogenation of CO* to CHO*. The dissociation of CHO* to form CH* and O* was identified as the rate limiting step for CH4 formation, while the rate limiting step for CO production through the reverse water gas shift reaction was identified as CO* desorption. Based on a scaling relations analysis of competing CHO* dissociation and CO* desorption, O* adsorption energy was found to be an effective descriptor of differences in selectivity between CO and CH4 production previously observed on late-transition metal catalysts. These mechanistic insights provide critical information to guide the design of catalysts with tunable selectivity for CO2 reduction by H-2 at atmospheric pressure. (C) 2016 Elsevier Inc. All rights reserved.
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