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利用光热效应增强肖特基结上光催化水分解与选择性苯甲醇氧化的耦合。

Utilizing Photothermal Effect Enhances Photocatalytic Water Splitting Coupled with Selective Benzyl Alcohol Oxidation over Schottky Junctions.

作者信息

Sun Bojing, Ye Mengjia, Xu Yachao, Jiang Ying, Hou Dongfang, Qiao Xiu-Qing, Wang Meidi, Du Yunchen, Li Dong-Sheng

机构信息

College of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, Hubei, 443002, P. R. China.

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.

出版信息

Adv Sci (Weinh). 2025 Jul;12(26):e2501931. doi: 10.1002/advs.202501931. Epub 2025 Apr 11.

Abstract

As is well known, there are problems such as low utilization rate of photogenerated holes and resource consumption of sacrificial agent in solar-driven photocatalytic water splitting to hydrogen technology. Herein, WC quantum dots decorated defective ZnInS nanosheets (DZIS/WCQDs) dual-functional photocatalysts are fabricated. Its unique Schottky junctions and photothermal effect significantly promote the separation and transport efficiency of photogenerated carriers, as well as achieving synergistic enhancement of photocatalytic water splitting coupled with selective oxidation of benzyl alcohol (BA). Moreover, the photothermal effect can slowly induce the decomposition of HO to produce ·OH, and the low concentration ·OH and photogenerated holes continuously generated in situ can directly and rapidly attack the αC─H bond of BA to improve benzaldehyde (BAD) conversion rate and selectivity. Consequently, DZIS/WCQDs composites exhibit a surprising conversion rate and selectivity of 85.34% and 96.53% for BAD, and outstanding H and BAD evolution rates of 12.58 and 10.53 mmol g h without sacrificial agent and co-catalyst. Notably, combining the production rate and selectivity of products, the DZIS/WCQDs is the optimal catalyst material at present. This work opens up a green and carbon free effective path to solve the problems of low efficiency and high cost of photocatalytic hydrogen production.

摘要

众所周知,在太阳能驱动的光催化水分解制氢技术中,存在光生空穴利用率低和牺牲剂资源消耗等问题。在此,制备了WC量子点修饰的缺陷ZnInS纳米片(DZIS/WCQDs)双功能光催化剂。其独特的肖特基结和光热效应显著提高了光生载流子的分离和传输效率,同时实现了光催化水分解与苯甲醇(BA)选择性氧化的协同增强。此外,光热效应可缓慢诱导HO分解产生·OH,原位持续产生的低浓度·OH和光生空穴可直接快速攻击BA的αC─H键,提高苯甲醛(BAD)的转化率和选择性。因此,DZIS/WCQDs复合材料对BAD的转化率和选择性分别达到了惊人的85.34%和96.53%,在无牺牲剂和助催化剂的情况下,H和BAD的产率分别高达12.58和10.53 mmol g h。值得注意的是,综合产物的产率和选择性来看,DZIS/WCQDs是目前最优的催化剂材料。这项工作为解决光催化制氢效率低和成本高的问题开辟了一条绿色、无碳的有效途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1ded/12245034/feade5e94af9/ADVS-12-2501931-g002.jpg

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