Journal
ACS CATALYSIS
Volume 6, Issue 6, Pages 3826-3833Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b00666
Keywords
dry reforming of methane; syngas; pyrochlore; steady-state isotopic transient kinetic analysis; reaction mechanism; DFT
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Funding
- Center for Atomic Level Catalyst Design, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001058]
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Increases in worldwide methane production from biological and fossil sources have led to an increased level of interest in the dry reforming of methane (DRM) to produce syngas. Experimental efforts have shown that select pyrochlore materials, such as the Rh-substituted lanthanum zirconate pyrochlore (LRhZ), are catalytically active for DRM, exhibit long-term thermal stability, and resist deactivation. This work seeks to allow further catalyst improvements by elucidating surface reaction kinetics via steady-state isotopic transient kinetic analysis (SSITKA) of dry reforming on the LRhZ pyrochlore. Isotopically labeled CH4 and CO2 were used in multiple SSITKA experiments to elucidate the migration of carbon atoms to product species. Short surface residence times at 650 and 800 degrees C (<0.6 s) were observed for DRM intermediates involved in reversible reactions, and the participation of all surface metal atoms as active sites for DRM, not only Rh, is suggested. Isotopic responses and kinetic isotope effects are explained using reaction mechanism details derived from density functional theory studies of the surface reactions.
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