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Understanding the relationship of competitive adsorption between reactants is the prerequisite for high activity and selectivity in heterogeneous catalysis, especially the difference between the adsorption energies (E-ads) of two reactive intermediates in Langmuir-Hinshelwood (L-H) models. Using oxidative dehydrogenation of hydrogen sulfide (H2S-ODH) as a probe, we develop various metal single atoms on nitrogen-doped carbon (M-NDC) catalysts for controlling E-ads-H2S, E-ads-O-2 and investigating the difference in activity and selectivity. Combining theoretical and experimental results, a Sabatier relationship between the catalytic performance and E-ads-O-2/E-ads-H2S emerges. Mn-NDC as the optimal catalyst shows excellent H2S conversion (>90 %) and sulfur selectivity (>90 %) in a wide range of O-2 concentrations over 100 h. Such a high-efficiency performance is attributed to appropriate E-ads-H2S and E-ads-O-2 on Mn-N-4 sites, boosting redox cycle between Mn2+ and Mn3+, as well as preferential formation of sulfur. This work provides a fundamental guidance for designing Sabatier optimal catalysts in L-H models.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN: 1433-7851
Year: 2024
Issue: 7
Volume: 64
1 6 . 1 0 0
JCR@2023
Cited Count:
SCOPUS Cited Count: 1
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
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