文献类型：期刊文献

英文题名：Modification approaches of mesoporous carbon aerogels for room-temperature H2S catalytic oxidation: base-loading vs. N-doping

作者：Chen, Shengwei[1];Zhang, Yu[1];Dong, Qi[1];Ma, Cheng[4];Qiao, Wenming[5];Wang, Jitong[1,2];Ling, Licheng[3]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Guangxi Univ, Univ Engn Res Ctr Green Chem New Mat, Sch Chem & Chem Engn, Nanning 530004, Guangxi, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Specially Funct Polymer Mat & Related Tech, Minist Educ, 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;[5]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：399

外文期刊名：SEPARATION AND PURIFICATION TECHNOLOGY

收录：;EI(收录号：20261920665592);WOS:【SCI-EXPANDED(收录号:WOS:001768536400001)】；

基金：This work is financially supported by the National Natural Science Foundation of China (Nos. U21A2060 and 22178116) and the Funda-mental Research Funds for the Central Universities (No. JKD01251701) .

语种：英文

外文关键词：Hydrogen sulfide; Catalytic oxidation; Carbon aerogel; Mesoporous material; Oxidation mechanism

摘要：Catalytic oxidation of hydrogen sulfide (H2S) at room temperature enables deep desulfurization and efficient recovery of elemental sulfur. Base-loading and N-doping are major modification strategies for carbon-based catalysts, while comparative research on their respective roles in carbon substrates and basic sites remains insufficient. Herein, silica-nanocasting on agarose hydrogel is adopted to fabricate highly mesoporous carbon aerogels with the modification of MgO-loading (MCAs) or urea co-pyrolysis (NCAs). Precise MgO regulation and ultra-high N doping of 23.1 wt% enhance aerogels to achieve excellent sulfur capacities of 3.38 and 0.90 g H2S g-1 depends only on nitrogen doping content. MgO-modified carbon alleviates sulfur blockage via water refreshing theory, yet its strong O2 activation capacity easily induces overoxidation. Nitrogen-doped carbon features mild oxygen activation, but suffers active site loss from strong S8 adsorption. DFT calculations indicate that H2S adsorption on the MgO surface is weak, whereas its dissociation energy barrier is extremely low. Pyrrolic and pyridinic N exhibit completely opposite behavior toward H2S compared with MgO. This study elucidates the catalytic oxidation mechanisms of the two modification strategies, providing a solid foundation for integrating their advantages to construct efficient desulfurization catalysts. cat, respectively. Performance of MCAs is constrained by pore volume and loading, while that of NCAs