Abstract
Ethane direct dehydrogenation (EDH) is of great importance for shale gas utilization. However, the development of highly active and stable catalyst is still challenge in this process. Here, to guide the establishment of a desired Rh-based catalyst for EDH to ethylene, fifteen catalysts RhxM (M=Cu, Ag, Au) (x=1, 2, 3, 6, 9) are designed and their catalytic performance for EDH are systematically studied by using density functional theory calculations. The computational results disclose that the aggregation form of active Rh atoms (ensemble effect) dominates the catalytic performance, rather than the d-band center, electron transfer and the effects of the second metal substrate. The catalysts Rh1Cu, Rh1Au, and Rh2Ag show the best catalytic performance among the catalysts with different metal substrate. Typically, the low-cost catalyst Rh1Cu with surface single-atom Rh in the non-noble metal Cu not only performs improved activity and selectivity for forming ethylene but also resists the coking. Interestingly, the catalyst Rh3M (M=Cu, Ag, Au) has poor C2H4 selectivity and coking resistance due to itself ensemble effect. This study gives a theoretical guidance for regulating the catalytic performance through the ensemble effect of active site metal atoms in ethane direct dehydrogenation.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.