Mengzhen Ren , Tianfu Liu , Yuanyuan Dong , Zheng Li , Jiaxin Yang , Zhenheng Diao , Hongjin Lv , Guo-Yu Yang
{"title":"利用耦合 CdS 纳米棒和含 Ni 的聚氧化金属酸盐将噻吩酚近乎统一地光催化脱氢偶联为二硫化物和氢气","authors":"Mengzhen Ren , Tianfu Liu , Yuanyuan Dong , Zheng Li , Jiaxin Yang , Zhenheng Diao , Hongjin Lv , Guo-Yu Yang","doi":"10.1016/S1872-2067(24)60025-2","DOIUrl":null,"url":null,"abstract":"<div><p>Simultaneously harnessing the photogenerated electrons and holes to convert thiols into the value-added disulfides with the concomitant formation of H<sub>2</sub> represents a highly promising strategy for maximizing the conversion of solar energy into chemical energy. Herein, we report an effective catalytic system comprising CdS nanorods (NRs) and Ni-containing polyoxometalate (Na<sub>6</sub>K<sub>4</sub>[Ni<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>(PW<sub>9</sub>O<sub>34</sub>)<sub>2</sub>] (Ni<sub>4</sub>P<sub>2</sub>)) (Ni<sub>4</sub>P<sub>2</sub>/CdS), which exhibited efficient photocatalytic activities towards the near-unity dehydrocoupling of 4-methoxythiophenol (4-MTP) into disulfide and H<sub>2</sub> evolution. The photooxidative dehydrocoupling of 4-MTP can be finished after 4 h photocatalysis, leading to 98.39% conversion of 4-MTP with the yield of disulfide and H<sub>2</sub> reaching 24.45 and 25.96 μmol, respectively. The Ni<sub>4</sub>P<sub>2</sub>/CdS catalytic system also showed good photocatalytic recycling stability. Comprehensive experimental and characterization results indicated that the synergistic cooperation between CdS NRs and Ni<sub>4</sub>P<sub>2</sub> facilitated the separation and migration of the photogenerated electron-hole pairs, thereby improving the photocatalytic dehydrocoupling of 4-MTP to disulfide coupling with hydrogen production.</p></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 312-321"},"PeriodicalIF":15.7000,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Near-unity photocatalytic dehydrocoupling of thiophenols into disulfides and hydrogen using coupled CdS Nanorods and Ni-containing polyoxometalate\",\"authors\":\"Mengzhen Ren , Tianfu Liu , Yuanyuan Dong , Zheng Li , Jiaxin Yang , Zhenheng Diao , Hongjin Lv , Guo-Yu Yang\",\"doi\":\"10.1016/S1872-2067(24)60025-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Simultaneously harnessing the photogenerated electrons and holes to convert thiols into the value-added disulfides with the concomitant formation of H<sub>2</sub> represents a highly promising strategy for maximizing the conversion of solar energy into chemical energy. Herein, we report an effective catalytic system comprising CdS nanorods (NRs) and Ni-containing polyoxometalate (Na<sub>6</sub>K<sub>4</sub>[Ni<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>(PW<sub>9</sub>O<sub>34</sub>)<sub>2</sub>] (Ni<sub>4</sub>P<sub>2</sub>)) (Ni<sub>4</sub>P<sub>2</sub>/CdS), which exhibited efficient photocatalytic activities towards the near-unity dehydrocoupling of 4-methoxythiophenol (4-MTP) into disulfide and H<sub>2</sub> evolution. The photooxidative dehydrocoupling of 4-MTP can be finished after 4 h photocatalysis, leading to 98.39% conversion of 4-MTP with the yield of disulfide and H<sub>2</sub> reaching 24.45 and 25.96 μmol, respectively. The Ni<sub>4</sub>P<sub>2</sub>/CdS catalytic system also showed good photocatalytic recycling stability. Comprehensive experimental and characterization results indicated that the synergistic cooperation between CdS NRs and Ni<sub>4</sub>P<sub>2</sub> facilitated the separation and migration of the photogenerated electron-hole pairs, thereby improving the photocatalytic dehydrocoupling of 4-MTP to disulfide coupling with hydrogen production.</p></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":\"61 \",\"pages\":\"Pages 312-321\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-06-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724600252\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600252","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Near-unity photocatalytic dehydrocoupling of thiophenols into disulfides and hydrogen using coupled CdS Nanorods and Ni-containing polyoxometalate
Simultaneously harnessing the photogenerated electrons and holes to convert thiols into the value-added disulfides with the concomitant formation of H2 represents a highly promising strategy for maximizing the conversion of solar energy into chemical energy. Herein, we report an effective catalytic system comprising CdS nanorods (NRs) and Ni-containing polyoxometalate (Na6K4[Ni4(H2O)2(PW9O34)2] (Ni4P2)) (Ni4P2/CdS), which exhibited efficient photocatalytic activities towards the near-unity dehydrocoupling of 4-methoxythiophenol (4-MTP) into disulfide and H2 evolution. The photooxidative dehydrocoupling of 4-MTP can be finished after 4 h photocatalysis, leading to 98.39% conversion of 4-MTP with the yield of disulfide and H2 reaching 24.45 and 25.96 μmol, respectively. The Ni4P2/CdS catalytic system also showed good photocatalytic recycling stability. Comprehensive experimental and characterization results indicated that the synergistic cooperation between CdS NRs and Ni4P2 facilitated the separation and migration of the photogenerated electron-hole pairs, thereby improving the photocatalytic dehydrocoupling of 4-MTP to disulfide coupling with hydrogen production.
期刊介绍：
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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