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一维半导体光催化剂中分子助催化剂与异质结的协同效应助力强劲且高效的太阳能制氢

Synergistic Effect of a Molecular Cocatalyst and a Heterojunction in a 1 D Semiconductor Photocatalyst for Robust and Highly Efficient Solar Hydrogen Production.

作者信息

Jiang Daochuan, Irfan Rana Muhammad, Sun Zijun, Lu Dapeng, Du Pingwu

机构信息

Key Laboratory of Materials for Energy Conversion, Chinese Academy of Sciences, Department of Materials Science and Engineering, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, 96 Jinzhai Road, 230026, Hefei, Anhui Province, P.R. China.

出版信息

ChemSusChem. 2016 Nov 9;9(21):3084-3092. doi: 10.1002/cssc.201600871. Epub 2016 Oct 12.

DOI:10.1002/cssc.201600871
PMID:27730758
Abstract

Photocatalytic production of hydrogen by water splitting is a promising pathway for the conversion of solar energy into chemical energy. However, the photocatalytic conversion efficiency is often limited by the sluggish transfer of the photogenerated charge carriers, charge recombination, and subsequent slow catalytic reactions. Herein, we report a highly active noble-metal-free photocatalytic system for hydrogen production in water. The system contains a water-soluble nickel complex as a molecular cocatalyst and zinc sulfide on 1D cadmium sulfide as the heterojunction photocatalyst. The complex can efficiently transport photogenerated electrons and holes over a heterojunction photocatalyst to hamper charge recombination, leading to highly improved catalytic efficiency and durability of a heterojunction photocatalyst- molecular cocatalyst system. The results show that under optimal conditions, the average apparent quantum yield was approximately 58.3 % after 7 h of irradiation with monochromatic 420 nm light. In contrast, the value is only 16.8 % if the molecular cocatalyst is absent. Such a remarkable performance in a molecular cocatalyst-based photocatalytic system without any noble metal loading has, to the best of our knowledge, not been reported to date.

摘要

通过光催化水分解制氢是将太阳能转化为化学能的一条很有前景的途径。然而,光催化转化效率常常受到光生载流子转移缓慢、电荷复合以及随后缓慢的催化反应的限制。在此,我们报道了一种用于水中制氢的高活性无贵金属光催化体系。该体系包含一种水溶性镍配合物作为分子助催化剂以及一维硫化镉上的硫化锌作为异质结光催化剂。该配合物能够在异质结光催化剂上高效传输光生电子和空穴,从而抑制电荷复合,使得异质结光催化剂 - 分子助催化剂体系的催化效率和耐久性得到显著提高。结果表明,在最佳条件下,用420 nm单色光照射7小时后,平均表观量子产率约为58.3%。相比之下,如果没有分子助催化剂,该值仅为16.8%。据我们所知,在没有任何贵金属负载的基于分子助催化剂的光催化体系中,如此卓越的性能至今尚未见报道。

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