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Cu/Biochar Bifunctional Catalytic Removal of COS and H2S:H2O Dissociation and CuO Anchoring Enhanced by Pyridine N
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2024-03-01 , DOI: 10.1021/acs.est.3c08914 Xiang Li 1 , Xueqian Wang 1 , Li Yuan 1 , Langlang Wang 1 , Yixing Ma 1 , Rui Cao 1 , Yibing Xie 1 , Yiran Xiong 1 , Ping Ning 1
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2024-03-01 , DOI: 10.1021/acs.est.3c08914 Xiang Li 1 , Xueqian Wang 1 , Li Yuan 1 , Langlang Wang 1 , Yixing Ma 1 , Rui Cao 1 , Yibing Xie 1 , Yiran Xiong 1 , Ping Ning 1
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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·g–1 and enhanced the turnover frequency of H2S from 2.50 × 10–4 to 5.35 × 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.
中文翻译：
Cu/生物炭双功能催化去除 COS 和 H2S：吡啶 N 增强 H2O 解离和 CuO 锚定
需要经济和环境友好的策略来促进通过水解去除硫化羰（COS）和通过氧化去除硫化氢（H 2 S）的双功能催化去除。氮掺杂被认为是一种有效的策略，但氮掺杂剂在催化剂中的本质和内在作用仍不清楚。在此，Cu/生物炭退火过程中尿素和生物炭的结合产生了吡啶N，这将催化剂的COS/H 2 S组合容量从260.7增加到374.8 mg·g –1 ，并将H 2 S的周转频率从2.50提高。 × 10 –4至 5.35 × 10 –4 s –1 。吡啶N的亲核性质增强了催化剂的中等碱性位点，使得质子的攻击和强烈的H 2 O解离成为可能。此外，吡啶 N 还形成锚定 CuO 的空腔位点，改善 Cu 分散性并产生更多活性氧。通过对吡啶 N 诱导的双功能催化在微氧和潮湿的气氛中去除 COS/H 2 S 提供了独到的见解，本研究为硫降解中进一步的 C=S 和 C-S 键断裂提供了有价值的指导。含有污染物。
更新日期：2024-03-01
中文翻译：
Cu/生物炭双功能催化去除 COS 和 H2S：吡啶 N 增强 H2O 解离和 CuO 锚定
需要经济和环境友好的策略来促进通过水解去除硫化羰（COS）和通过氧化去除硫化氢（H 2 S）的双功能催化去除。氮掺杂被认为是一种有效的策略，但氮掺杂剂在催化剂中的本质和内在作用仍不清楚。在此，Cu/生物炭退火过程中尿素和生物炭的结合产生了吡啶N，这将催化剂的COS/H 2 S组合容量从260.7增加到374.8 mg·g –1 ，并将H 2 S的周转频率从2.50提高。 × 10 –4至 5.35 × 10 –4 s –1 。吡啶N的亲核性质增强了催化剂的中等碱性位点，使得质子的攻击和强烈的H 2 O解离成为可能。此外，吡啶 N 还形成锚定 CuO 的空腔位点，改善 Cu 分散性并产生更多活性氧。通过对吡啶 N 诱导的双功能催化在微氧和潮湿的气氛中去除 COS/H 2 S 提供了独到的见解，本研究为硫降解中进一步的 C=S 和 C-S 键断裂提供了有价值的指导。含有污染物。
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