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硫化物固溶体纳米分支从纯水和空气中实现压电催化和光催化析氢过氧化物

Piezocatalytic and Photocatalytic Hydrogen Peroxide Evolution of Sulfide Solid Solution Nano-Branches from Pure Water and Air.

作者信息

Lin Sen, Wang Qi, Huang Hongwei, Zhang Yihe

机构信息

Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing, 100083, P. R. China.

出版信息

Small. 2022 May;18(19):e2200914. doi: 10.1002/smll.202200914. Epub 2022 Apr 11.

DOI:10.1002/smll.202200914
PMID:35403802
Abstract

Hydrogen peroxide (H O ) as a useful chemical has a wide range of applications, and the development of efficient semiconducting materials for H O production is deemed as a promising strategy to realize the energy conversion. In this paper, Cd Zn S (x = 0, 0.1, 0.3, 0.5, 0.7, 0.9, 1) nano-branches are fabricated and the piezocatalytic and photocatalytic H O evolution performance are studied. Under ultrasound condition, the H O yield of as-synthesized solid solutions is all higher than those of pristine ZnS and CdS, and optimal evolution rate achieves 21.9 µmol g h for Cd Zn S without any sacrificial agent, while it is increased to 151.6 µmol g h under visible light irradiation. The piezo/photoelectrochemical tests, piezoresponse force microscopy (PFM), and computational simulation reveal that the nano-branch structure benefits the mechanical energy conversion more, favoring the H O evolution for Cd Zn S, and a higher concentration of charge carriers is generated in photocatalysis. The active radical trapping and in situ electron spin resonance (ESR) experiments demonstrate that both of the H O generation pathways are originated from oxygen reduction by the sequential two-step single-electron reaction. This work opens a door for promoting the H O production from nanostructure and solid solution design.

摘要

过氧化氢(H₂O₂)作为一种有用的化学品具有广泛的应用,开发用于生产H₂O₂的高效半导体材料被认为是实现能量转换的一种有前景的策略。本文制备了CdₓZn₁₋ₓS(x = 0、0.1、0.3、0.5、0.7、0.9、1)纳米分支,并研究了其压电催化和光催化产H₂O₂的性能。在超声条件下,合成的固溶体的H₂O₂产率均高于原始ZnS和CdS,对于Cd₀.₅Zn₀.₅S,在没有任何牺牲剂的情况下,最佳产率达到21.9 μmol g⁻¹ h⁻¹,而在可见光照射下,产率提高到151.6 μmol g⁻¹ h⁻¹。压电/光电化学测试、压电响应力显微镜(PFM)和计算模拟表明,纳米分支结构更有利于机械能转换,有利于CdₓZn₁₋ₓS产H₂O₂,并且在光催化过程中产生更高浓度的电荷载流子。活性自由基捕获和原位电子自旋共振(ESR)实验表明,两种H₂O₂生成途径均源于通过连续两步单电子反应的氧还原。这项工作为通过纳米结构和固溶体设计促进H₂O₂的生产打开了一扇门。

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