Ye Hanfeng, Xing Wandong, Zhao Fei, Wang Jiali, Yang Can, Hou Yidong, Zhang Jinshui, Yu Jimmy C, Wang Xinchen
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108, P. R. China.
Department of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong, 999077, P. R. China.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202419630. doi: 10.1002/anie.202419630. Epub 2024 Dec 10.
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) of two reactive intermediates in Langmuir-Hinshelwood (L-H) models. Using oxidative dehydrogenation of hydrogen sulfide (HS-ODH) as a probe, we develop various metal single atoms on nitrogen-doped carbon (M-NDC) catalysts for controlling E-HS, E-O and investigating the difference in activity and selectivity. Combining theoretical and experimental results, a Sabatier relationship between the catalytic performance and E-O/E-HS emerges. Mn-NDC as the optimal catalyst shows excellent HS conversion (>90 %) and sulfur selectivity (>90 %) in a wide range of O concentrations over 100 h. Such a high-efficiency performance is attributed to appropriate E-HS and E-O on Mn-N sites, boosting redox cycle between Mn and Mn, as well as preferential formation of sulfur. This work provides a fundamental guidance for designing Sabatier optimal catalysts in L-H models.
