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Hierarchically porous, N-defect enriched C-nanosheets boost the H2S selective oxidation to elemental sulfur

Journal 2023 · IF 22.1 · 发表于 2023 年 11 月 11 日
作者: Shiyan Li,Hongquan Fu,Xingshuai Zhang,Xu Liu,Giulia Tuci,Giuliano Giambastiani,Cuong Pham-Huu,Yuefeng Liu
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摘要

H 2 S selective oxidation to elemental sulfur (S 8 ) is a typical reaction where the mass product diffusion ( e.g ., S 8 ) through the catalytic bed is crucial as well as the reagents accessibility ( e.g ., H 2 S, O 2 ) to the active sites. The NaNO 3 -assisted pyrolysis of polyacrylamide was applied to synthesize defect-enriched N-doped carbon nanosheets with thickness up to c.a. 2 nm, featured by fully accessible and highly interconnected pores, for boosting the H 2 S selective oxidation process. The PAM-0.3-700 sample has revealed an unprecedented desulfurization activity with sulfur formation rate of 1165 g sulfur kg cat. −1 h −1 , other than a remarkable stability (>80 h). Experimental and theoretical studies have unveiled the critical role of edge sites containing unpaired electrons and nitrogen species with respect to the material aptitude towards O 2 dissociation and HS - activation. The material in presence of a highly interconnected porous network facilitates the reactants/product diffusion especially for catalysis operated under harsh experimental conditions.

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