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在用于高效光催化析氢的硫化铜/硫化锌镉异质纳米片中直接观察Z型路线

Direct Observation of Z-Scheme Route in CuS/ZnCdS Heteronanoplates for Highly Efficient Photocatalytic Hydrogen Evolution.

作者信息

Lian Zichao, Qu Minghan, Xiao Han, Wang Lihui, Wu Hanxiang, Zi Jiangzhi, Wang Wei, Li Hexing

机构信息

School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai, 200093, P. R. China.

Department of Pharmacology & Toxicology and Department of Chemistry & Biochemistry, University of Arizona, Tucson, AZ, 85721, USA.

出版信息

Small. 2024 Aug;20(32):e2400611. doi: 10.1002/smll.202400611. Epub 2024 Mar 15.

DOI:10.1002/smll.202400611
PMID:38488704
Abstract

Although photocatalytic hydrogen production from water holds great potential as a renewable and sustainable energy alternative, the practical application of the technology demands cost-effective, simple photocatalytic systems with high efficiency in hydrogen evolution reaction (HER). Herein, the synthesis and characterization of CuS/ZnCdS heterostructured nanoplates (CuS/ZnCdS HNPs) as a high photocatalytic system are reported. The cost-effective, hierarchical structures are easily prepared using the CuS NPs as the seed by the epitaxial growth of the ZnCdS nanocrystals (NCs). The CuS/ZnCdS without the noble metal cocatalyst exhibits a high HER rate of 61.7 mmol g h, which is 8,014 and 17 times higher than that of CuS and ZnCdS, respectively, under visible light irradiation. The apparent quantum yield (AQY) of CuS/ZnCdS reaches 67.9% at 400 nm with the highest value so far in the reported ZnCdS-based photocatalysts. The excellent activity and stability of the CuS/ZnCdS are attributed to the formation of a strong internal electric field (IEF) and the Z-scheme pathway. The comprehensive experiments and theoretical calculations provide the direct evidences of the Z-scheme route. This work may offer a way for the design and development of efficient photocatalysts to achieve solar-to-chemical energy conversion at a practically useful level.

摘要

尽管光催化水制氢作为一种可再生且可持续的能源替代方案具有巨大潜力,但该技术的实际应用需要具备成本效益、简单且在析氢反应(HER)中具有高效率的光催化系统。在此,报道了作为高光催化系统的硫化铜/硫化锌镉(CuS/ZnCdS)异质结构纳米片(CuS/ZnCdS HNPs)的合成与表征。通过以硫化铜纳米颗粒(CuS NPs)为种子,利用硫化锌镉纳米晶体(NCs)的外延生长,可轻松制备出具有成本效益的分级结构。在可见光照射下,不含贵金属助催化剂的CuS/ZnCdS展现出61.7 mmol g⁻¹ h⁻¹的高HER速率,分别比CuS和ZnCdS高8014倍和17倍。CuS/ZnCdS在400 nm处的表观量子产率(AQY)达到67.9%,是迄今报道的基于硫化锌镉的光催化剂中的最高值。CuS/ZnCdS优异的活性和稳定性归因于强内建电场(IEF)的形成和Z型途径。综合实验和理论计算为Z型途径提供了直接证据。这项工作可能为设计和开发高效光催化剂以实现实际可用水平的太阳能到化学能转换提供一条途径。

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