Near-unity photocatalytic dehydrocoupling of thiophenols into disulfides and hydrogen using coupled CdS Nanorods and Ni-containing polyoxometalate

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI:10.1016/S1872-2067(24)60025-2

Mengzhen Ren , Tianfu Liu , Yuanyuan Dong , Zheng Li , Jiaxin Yang , Zhenheng Diao , Hongjin Lv , Guo-Yu Yang

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Abstract

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.

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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

同时利用光产生的电子和空穴将硫醇转化为高附加值的二硫化物，并同时形成 H2，是最大限度地将太阳能转化为化学能的一种极具前景的策略。在此，我们报告了一种由 CdS 纳米棒（NRs）和含 Ni- 的聚氧化金属盐（Na6K4[Ni4(H2O)2(PW9O34)2] (Ni4P2)）（Ni4P2/CdS）组成的有效催化体系，该催化体系在将 4-甲氧基苯硫酚（4-MTP）转化为二硫化物和 H2 演化过程中表现出高效的光催化活性。4-MTP 的光氧化脱氢偶联反应在光催化 4 小时后即可完成，4-MTP 的转化率达到 98.39%，二硫化物和 H2 的产率分别达到 24.45 和 25.96 μmol。Ni4P2/CdS 催化体系还表现出良好的光催化循环稳定性。综合实验和表征结果表明，CdS NRs 和 Ni4P2 之间的协同作用促进了光生电子-空穴对的分离和迁移，从而提高了 4-MTP 光催化脱氢偶联成二硫化物并产生氢气的能力。

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ethylenediamine

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CH4N2S

来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

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.