纳米异质结光催化剂制氢研究进展

催化学报 ›› 2017, Vol. 38 ›› Issue (8): 1295-1306.

纳米异质结光催化剂制氢研究进展

杜虹^a,b, 刘亚男^a, 申丛丛^a, 徐安武^a

a 中国科学技术大学合肥微尺度物质科学国家实验室纳米材料与化学研究部, 安徽合肥 230026;
b 新疆师范大学化学化工学院, 新疆乌鲁木齐 830054

收稿日期:2017-05-16 修回日期:2017-06-05 出版日期:2017-08-18 发布日期:2017-08-04
通讯作者: 徐安武
基金资助:
国家自然科学基金（51572253，21271165）；中国科学院合肥科学中心科研资助（2015SRG-HSC048）；国家自然科学基金委与荷兰科学研究院合作（51561135011）.

Nanoheterostructured photocatalysts for improving photocatalytic hydrogen production

Hong Du^a,b, Ya-Nan Liu^a, Cong-Cong Shen^a, An-Wu Xu^a

a Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, Anhui, China;
b College of Chemistry and Chemical Engineering, Xinjiang Normal University, Urumqi 830054, Xinjiang, China

Received:2017-05-16 Revised:2017-06-05 Online:2017-08-18 Published:2017-08-04
Supported by:
This work was supported by the National Natural Science Foundation of China (51572253, 21271165), Scientific Research Grant of Hefei Science Center of CAS (2015SRG-HSC048), and Cooperation between NSFC and Netherlands Organization for Scientific Research (51561135011).

摘要/Abstract

摘要：

随着世界经济的迅猛发展，人们生活水平飞速提高的同时，能源短缺和环境污染成为当前人类可持续发展过程中的两大严峻问题.氢作为一种能源载体，能量密度高，可储可运，且燃烧后唯一产物是水，不污染环境，被认为是今后理想的无污染可再生替代能源.20世纪60年代末，日本学者Fujishima和Honda发现光照n-型半导体TiO₂电极可导致水分解，使人们认识到了利用半导体光催化分解水制氢可直接将太阳能转化为氢能的可行性，利用半导体光催化分解水制氢逐渐成为能源领域的研究热点之一.然而，单相光催化材料的光生电子和空穴复合仍然严重，光催化制氢效率低，无法满足实际生产需要；另外，单相光催化材料不能同时具备较窄的禁带、较负的导带和较正的价带.
近年来，国内外学者在新型光催化材料的探索、合成和改性以及光催化理论等领域开展了大量研究工作.不断有不同种类的半导体材料被研究和发展为光催化分解水制氢催化材料.例如，具有可见光催化活性的阴、阳离子掺杂TiO₂，具有可见光下光解纯水能力的In_0.9Ni_0.9TaO₄，在256 nm紫外光辐照下量子效率达到56%的镧掺杂NaTaO₃，CdS以及（AgIn）_xZn_2（1-x）S₂等.在现有的光催化材料中，单相光催化材料可以通过掺杂、形貌控制合成、晶面控制合成、染料敏化和表面修饰等提高其光催化活性.复合型光催化材料则能通过组合不同电子结构的半导体材料并调控其光生载流子迁移获得优异的光催化制氢性能，大幅拓展了光催化制氢材料的研究范围和提升了光催化制氢性能.构建异质结能够有效提高光生电子-空穴分离效率，促使更多的光生电子参与光催化制氢反应，提高其氧化还原能力，从而提高其光催化制氢效率.
在I-型纳米异质结中，半导体A的价带高于半导体B，而导带则是前者高于后者，光照时，光生电子-空穴对的迁移速率是不同的，延长了光生电子的寿命，从而提高了材料的光催化活性.但是在I-型异质结中，电子和空穴都集中在B半导体上，这样光生电子-空穴对的复合几率仍然很高.Ⅱ-型异质结中电子和空穴的富集处各不相同，因此使用范围也更广泛一些.光辐照激发时，光生电子从半导体B的导带迁移到半导体A的导带上，而空穴则从半导体A的价带向半导体B的价带上转移，从而形成了载流子的空间隔离，有效抑制其复合.但是，在这个类型的异质结中，光生电子转移到了相对位置较低的导带，而空穴则转移到相对位置较高的价带，这样就降低了光生电子的还原能力和空穴的氧化能力.pn型异质结中，在两种半导体相互接触时，由于电子-空穴对的扩散作用，两种半导体的能带发生漂移，其中p型上移，n型下移.而且在两种半导体异质结的界面处会产生空间电荷层，在这个电荷层的作用下，在异质结界面上形成内建电场.在合适波长的光源辐照的条件下，两种半导体同时被激发，光生电子在内建电场的作用下，从p型半导体快速迁移到n型半导体上，而n型半导体中留在价带上的空穴则快速迁移到p型半导体上，这样光生电子-空穴对就得到了有效的分离.在以Z型载流子迁移为主导的异质结构材料中摈弃了中间媒介，通过控制界面的载流子迁移使低能量的光生电子与空穴直接复合保留高能量的光生电子-空穴，从而提高了材料的光催化效率.
本文介绍了纳米异质结光催化剂在设计合成方面的研究进展，总结了几种纳米异质结（I-型、Ⅱ-型、pn-型及Z-型）的光催化原理及其在制取氢气方面的研究进展，并展望了研究发展方向.期望本文能够加深研究者对该领域的理解，为今后高效光催化材料的设计提供帮助和指导.

关键词: 异质结, 导带, 价带, 电荷迁移, 光催化制氢

Abstract:

Rapid industrialization has accordingly increased the demand for energy. This has resulted in the increasingly severe energy and environmental crises. Hydrogen production, based on the photocatalytic water splitting driven by sunlight, is able to directly convert solar energy into a usable or storable energy resource, which is considered to be an ideal alternative energy source to assist in solving the energy crisis and environmental pollution. Unfortunately, the hydrogen production efficiency of single phase photocatalysts is too low to meet the practical requirements. The construction of heterostructured photocatalyst systems, which are comprised of multiple components or multiple phases, is an efficient method to facilitate the separation of electron-hole pairs to minimize the energy-waste, provide more electrons, enhance their redox ability, and hence improve the photocatalytic activity. We summarize the recent progress in the rational design and fabrication of nanoheterostructured photocatalysts. The heterojunction photocatalytic hydrogen generation systems can be divided into type-I, type-Ⅱ, pn-junction and Z-scheme junction, according to the differences in the transfer of the photogenerated electrons and holes. Finally, a summary and some of the challenges and prospects for the future development of heterojunction photocatalytic systems are discussed.

Key words: Heterojunction, Conduction band, Valence band, Charge transfer, Photocatalytic hydrogen production

杜虹, 刘亚男, 申丛丛, 徐安武. 纳米异质结光催化剂制氢研究进展[J]. 催化学报, 2017, 38(8): 1295-1306.

Hong Du, Ya-Nan Liu, Cong-Cong Shen, An-Wu Xu. Nanoheterostructured photocatalysts for improving photocatalytic hydrogen production[J]. Chinese Journal of Catalysis, 2017, 38(8): 1295-1306.

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