Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization

CHEMICAL ENGINEERING SCIENCE(2023)

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摘要
Selective catalytic oxidation of H2S into elemental sulfur has been recognized as the optimal route for H2S reutilization, but traditional metal catalysts show poor sulfur resistance. Herein, we report a solvent-free route for designing nitrogen and defects co-doped, ordered mesoporous carbons (ND-OMCs) from co-assembly of block copolymer template with nitrogen-containing oligomers and silica defects directing agent. Through thermal curing, carbonization and etching of silica, the microporosity tandem ordered mesopores, abundant nitrogen sites (6.13 wt%) and structural defects were introduced into ND-OMCs. The ND-OMCs were successfully applied as efficient and long-lived metal-free catalysts for H2S selective oxidation to sulfur, giving nearly 100 % H2S conversion and sulfur selectivity at only 150 degrees C. Their remark-able activities of ND-OMCs can be well-maintained over 157 h of continuous reaction, exhibiting the sul-fur capacity as high as 3295 mg/g, which were much better than mostly desulfurizes such as commercial Fe2O3, g-C3N4, and nitrogen-containing, ordered mesoporous carbons.(c) 2023 Elsevier Ltd. All rights reserved.
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关键词
Sustainable design,Ordered mesoporosity,Nitrogen-doped porous carbon,Structural defects,H2S catalytic reutilization
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