With natural gas becoming a plentiful resource and CO2 impacting climate, developing methane dry reforming catalysts that operate at lower temperatures with more ideal product distributions (1:1 H2:CO) is of significant interest to the community. Methane dry reforming exhibits many challenges due to ineffective carbon oxidation that leads to coke formation and the reverse water-gas shift reaction that consumes oxygen and hydrogen via H2O formation. Common metal (TM) and TM+TM alloys often suffer from coke deposition and require high temperature reaction environments to limit reverse water-gas shift. On the other hand, ideal catalyst surface chemistry would enable C-H activation and oxidation of CHx/C for CO production at lower temperature while simultaneously controlling the fate of atomic H to limit the hydrogenation of O/OH to form H2O and promote H2 formation. Intermetallic compounds (IMCs) have been found to present a new spectrum of surface chemistry towards C, O, and H that may be appropriate for dry reforming catalyst design. However, the most ideal surface chemistry for the reaction is still unclear. This study focuses on mapping the catalytic surface chemistry of IMCs to produce a clear pathway forward for catalyst design. Computational surface science studies have helped to isolate critical surface reactivity needed for the reaction and IMC formulations that may inhibit RWGS activity while still achieving high rates of C-H activation and CHx/C oxidation. Preliminary experimental results focusing on IMCs predicted to improve DRM performance will also be reviewed.

Insights into controlling the surface chemistry of the dry reforming of methane reaction over intermetallic compounds

ACS Fall 2021

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