Cu/Biochar Bifunctional Catalytic Removal of COS and H2S:H2O Dissociation and CuO Anchoring Enhanced by Pyridine N

ENVIRONMENTAL SCIENCE & TECHNOLOGY(2024)

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摘要
Economic and environmentally friendly strategies are needed to promote the bifunctional catalytic removal of carbonyl sulfide (COS) by hydrolysis and hydrogen sulfide (H2S) by oxidation. N doping is considered to be an effective strategy, but the essential and intrinsic role of N dopants in catalysts is still not well understood. Herein, the conjugation of urea and biochar during Cu/biochar annealing produced pyridine N, which increased the combined COS/H2S capacity of the catalyst from 260.7 to 374.8 mg center dot g(-1) and enhanced the turnover frequency of H2S from 2.50 x 10(-4) to 5.35 x 10(-4) s(-1). The nucleophilic nature of pyridine N enhances the moderate basic sites of the catalyst, enabling the attack of protons and strong H2O dissociation. Moreover, pyridine N also forms cavity sites that anchor CuO, improving Cu dispersion and generating more reactive oxygen species. By providing original insight into the pyridine N-induced bifunctional catalytic removal of COS/H2S in a slightly oxygenated and humid atmosphere, this study offers valuable guidance for further C= S and C-S bond-breaking in the degradation of sulfur-containing pollutants.
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biochar-based bifunctional catalyst,pyridine N,-OH generation,CuO dispersion,COS hydrolysis,H2S oxidation,blast furnace gas
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