文献类型：期刊文献

英文题名：Surface chemical modulation of nitrogen-doped microporous carbon for efficient removal of H2S and CO2: The effect of nitrogen functionality

作者：Ma, Yongping[1];Xu, Yan[2];Liu, Fan[1];Zhang, Yankai[1];Wang, Jitong[1,2]

机构：[1]Guangxi Univ, Sch Chem & Chem Engn, Guangxi Key Lab Petrochem Resource Proc & Proc Int, Nanning 530004, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China

年份：2025

卷号：387

外文期刊名：MICROPOROUS AND MESOPOROUS MATERIALS

收录：;EI(收录号：20250417759342);WOS:【SCI-EXPANDED(收录号:WOS:001410633200001)】；

基金：Acknowledgments This work is financially supported by the National Natural Science Foundation of China (22178116) , the Natural Science Foundation of Shanghai Municipality (No. 22ZR1417400) .

语种：英文

外文关键词：CO2 adsorption; H2S removal; Nitrogen doping; Surface chemical modulation; DFT simulation

摘要：The removal of hydrogen sulfide (HAS) and carbon dioxide (COA) is of paramount importance for mitigating environmental pollution. However, due to the difficulty in accurately controlling the surface chemistry, the performance of carbon materials in the simultaneous removal of HAS and COA remains relatively limited. Herein, nitrogen-doped microporous carbon with well-developed pore structure was prepared through a combination of hydrothermal synthesis and molten salt method. The impact of nitrogen-doped surface chemistry on the removal performance for HAS and COA at room temperature was primarily studied. Owing to its abundant micropores and ultramicropores, the material possesses sufficient basic sites that can effectively remove COA. Pyrrolic nitrogen serves as the primary basic site during COA adsorption, which exhibits an excellent COA adsorption capacity of 136.97 mg COA/g. The high nitrogen content provides a strongly alkaline environment conducive to the dissociation of HAS on the carbon surface, with pyrrolic nitrogen being the main basic site during the catalytic oxidation of HAS. The large pore volume offers sufficient storage space for desulfurization products, enabling a sulfur capacity of 2.56 g HAS/g. DFT calculations reveal that pyrrolic nitrogen undergoes the largest change in charge before and after the adsorption of COA and HAS, due to its strong adsorption effect on both gases. In the presence of both COA and HAS, competition for active sites leads to a decline in the removal performance for both gases. This work holds significant implications for the design of materials for the simultaneous removal of COA and HAS.