Efficient catalytic removal of COS and H_(2)S over graphitized 2D micro-meso-macroporous carbons endowed with ample nitrogen sites synthesized via mechanochemical carbonization

查看全文 作　　者：Xun [1]Kan;Guanqing [1]Zhang;Yingying [1]Luo;Fujian [1]Liu;Yong [1]Zheng;Yihong [1]Xiao;Yanning [1]Cao;Chak-tong [1]Au;Shijing [1]Liang;Lilong [1]Jiang

机构地区：[1]National Engineering Research Center of Chemical Fertilizer Catalyst(NERC-CFC),School of Chemical Engineering,Fuzhou University,Fuzhou,350002,China

出　　处：《Green Energy & Environment》索引2022年第7卷第5期,共13页

基　　金：supported by the National Natural Science Foundation of China(22022804,21978052);the Natural Science Foundation for the Distinguished Young Scholar of Fujian Province(2020J06037);the National Key Research and Development Program of China(2018YFA0209304)。 摘　　要：Developing a suitable catalyst for the elimination of highly toxic carbonyl sulfide(COS)and hydrogen sulfide(H_(2)S) is of great significance in terms of industrial safety and environmental protection.We demonstrate here the facile synthesis of graphitized 2D micro-meso-macroporous carbons by one-step carbonization of a mixture of urea and glucose at 700–900℃.The as-synthesized graphitized catalysts,designated as 2DNHPC-x(x=urea/glucose mass ratio),are endowed with an ultra-high concentration(12.9–20.2 wt%)of stable and versatile nitrogen sites(e.g.pyrrole and pyridine)which are anchored on the surface via stable covalent bonding.As a result,the 2D-NHPC-x are active in catalytic hydrolysis of COS on pyrrolic N to H_(2)S,and the H_(2)S can be subsequently captured on pyridinic N and converted to elemental sulfur at ambient conditions over the same materials.Among the prepared catalysts,2D-NHPC-x can catalytically hydrolysize 91%of COS to H_(2)S at 30℃,whereas the conversion ratio over the common catalysts g-C_(3)N_(4)and Fe_(2)O_(3)are below 6.0%.Furthermore,these catalysts also exhibit H_(2)S conversion and sulfur selectivity of nearly 100%at 180℃with long-time durability,which is higher than those of the most reported carbonbased catalysts.In contrast,the H_(2)S capacities of activated carbon,ordered mesoporous carbons(OMC)and N-doped OMC are 3.9,1.5 and2.39 mmol g^(-1),respectively.Both the experimental and theoretical results are disclosed that 2D-NHPC-x are superior to the nitrogen-doped porous materials ever applied in simultaneous catalytic elimination of both COS and H_(2)S. 关键词：CARBONS catalytic endowed

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Efficient catalytic removal of COS and H_(2)S over graphitized 2D micro-meso-macroporous carbons endowed with ample nitrogen sites synthesized via mechanochemical carbonization

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