文献类型：期刊文献

英文题名：Water Film Theory-Guided Design of MgO@Carbon Nanoflowers for Room-Temperature H2S-Oxidation: Synergistic Effect Enabling Ultrahigh Carbon Utilization

作者：Chen, Shengwei[1];Liu, Chuanlei[1];Dong, Qi[1];Zhang, Yongzheng[1];Ma, Cheng[4];Qiao, Wenming[3];Sun, Hui[1,3];Wang, Jitong[1,2,3];Ling, Licheng[3]

机构：[1]East China Univ Sci & Technol, Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Guangxi Univ, Green Chem New Mat Engn Res Ctr Guangxi Coll & Uni, Sch Chem & Chem Engn, Nanning 530004, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Specially Funct Polymer Mat & Related Tech, Minist Educ, Shanghai 200237, Peoples R China

年份：2025

卷号：15

期号：16

起止页码：13787

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20261620502626);WOS:【SCI-EXPANDED(收录号:WOS:001537135900001)】；

基金：This work is financially supported by the National Natural Science Foundation of China (Nos. U21A2060 and 22178116) and the Fundamental Research Funds for the Central Universities (222201817001, 50321041918013, JKA01221601, and JKD01241701).

语种：英文

外文关键词：catalytic oxidation; hydrogen sulfide; molecularsimulation; nanoflower catalyst; water film theory

摘要：Extensive research has been conducted on the selective catalytic oxidation of hazardous H2S to elemental sulfur at room temperature using base-loaded carbon catalysts. However, practical applications of these catalysts are hindered by economic and environmental constraints associated with the complex synthesis and activation of functional carbon substrates. Understanding the synergistic mechanism between carbon and bases is crucial for developing innovative catalysts with low carbon content. Herein, molecular simulations were first employed to elucidate the adsorption preferences and reaction pathways within the water film theory, confirming the carbon-MgO interface as the active catalytic site. Furthermore, the ultrathin hierarchically porous carbon layer was demonstrated to effectively mitigate catalyst deactivation by maintaining reaction channels and facilitating product diffusion. Guided by the theoretical insights, nanoflower catalysts were successfully constructed with precisely controlled carbon coating content. Remarkably, MgO@C-0.1 with only 16.7 wt % carbon content exhibited an exceptional sulfur capacity of 4.32 g H2S g-1 cat. This unprecedented carbon utilization efficiency stems from interfacial carbon defects, enhanced mass transport through the ultrathin carbon layer, and abundant sulfur storage space outside nanosheets. This study provides fundamental design principles for exploiting the catalytic potential of carbon and offers inspiring perspectives for developing high-performance catalysts with low carbon footprint.