基于Ag<sub>3</sub>PO<sub>4</sub>的全固态Z型光催化体系研究进展

引用本文: 葛明, 李振路. 基于Ag₃PO₄的全固态Z型光催化体系研究进展[J]. 催化学报, 2017, 38(11): 1794-1803. doi: 10.1016/S1872-2067(17)62905-X shu

Citation: Ming Ge, Zhenlu Li. Recent progress in Ag₃PO₄-based all-solid-state Z-scheme photocatalytic systems[J]. Chinese Journal of Catalysis, 2017, 38(11): 1794-1803. doi: 10.1016/S1872-2067(17)62905-X shu

基于Ag₃PO₄的全固态Z型光催化体系研究进展

葛明 ^a,b, ,
李振路 ^a,

a 华北理工大学化学工程学院, 河北唐山 063210;
b 河北省环境光电催化材料重点实验室, 河北唐山 063210
基金项目:
河北省教育厅青年基金（QN2017115）；国家自然科学基金（51504079）.

摘要: 随着现代工业的迅猛发展，人类面临的能源危机和环境污染问题日益严重.光催化剂技术有望利用太阳能同时解决这两大问题，其关键在于设计高效的光催化体系.传统光催化材料TiO₂具有价廉、活性高及稳定性好等优点，然而其带隙宽（E_g=3.2 eV），仅能利用占太阳光谱约4%的紫外光，从而限制其利用太阳能.可见光占太阳光谱的40%以上，因此开发可见光响应的光催化材料成为光催化领域研究焦点.
2010年，叶金花课题组报道了Ag₃PO₄在可见光照射下可高效分解水产氧及降解水体中有机污染物，从而使其迅速成为研究热点.Ag₃PO₄是目前为止报道的光量子效率最高的可见光响应的催化材料，带隙能在2.3~2.5 eV范围内，其高效的光催化活性归结于其独特的电子结构利于光生电荷的分离及转移.然而，由于Ag₃PO₄本身易光蚀，稳定性差，必然限制其实际应用.近年来，为在进一步提升Ag₃PO₄活性的基础上增强稳定性，研究者通过多种方法对其进行修饰，包括贵金属沉积、碳材料修饰、负载及半导体异质复合等.相对于前面几种修饰方法，半导体复合相对高效且成本低.半导体复合主要构成Ⅱ型异质结构和Z型光催化体系.Ⅱ型异质结构由于内建电场的存在可以促进光生电荷的定向转移，从而提高光生电荷的分离效率，进而提高光催化活性.然而，这种电荷的定向迁移会降低光生电荷的氧化还原能力.
模拟绿色植物的光合作用过程，一种全固态Z型光催化体系应运而生，其是将两种导带和价带位置匹配的可见光驱动的催化剂分别作为光催化系统I （PS I）和光催化系统Ⅱ （PS Ⅱ），同时选用导电性能优良的材料（Ag，Au和RGO等）作为电子介体.可见光照条件下，PS I和PS Ⅱ均被激发产生电子和空穴，PS Ⅱ导带上的电子通过电子介质与PS I价带空穴复合，一方面抑制了PS I和PS Ⅱ本身电子和空穴的复合，另一方面保留了PS I导带电子的强还原性和PS Ⅱ价带空穴的强氧化性.另外，PS I和PS Ⅱ紧密结合形成具有准连续能级的固-固接触界面，PS Ⅱ导带上的电子直接与PS I价带空穴复合，形成无电子介体的直接Z型光催化体系.
Ag₃PO₄价带顶相对靠下，氧化能力强，往往作为PS Ⅱ组分，其与导带顶相对靠上的催化剂（PS I）构成Z型体系，这样Ag₃PO₄导带电子可与PS I的价带空穴复合，减弱电子对Ag₃PO₄本身的还原，提高其稳定性；另一方面，Ag₃PO₄价带空穴可参与氧化反应.基于Ag₃PO₄的Z型体系主要以Ag作为电子介体，归因于在制备及光催化过程中原位产生的少量Ag可直接作为电子介体.此外，还原氧化石墨烯（RGO）也可作为电子介体，并且其存在可进一步提高Ag₃PO₄的稳定性.需要指出的是，基于Ag的等离子体共振效应，Ag₃PO₄基等离子体Z型光催化体系也受到关注.
目前，Z型光催化体系处在发展阶段，必然存在一些问题，比如，Ⅱ型异质光催化体系与直接Z型光催化体系如何区分，有待进一步研究.另外，报道的基于Ag₃PO₄的Z型体系主要用来光催化降解水体中的有机污染物，催化剂的回收再利用受到限制，今后可开发磁性Ag₃PO₄基Z型体系，解决回收再利用的问题；另外，通过能带调控，可将基于Ag₃PO₄的Z型体系多用于光催化产氢、还原CO₂及处理有害气体.

关键词:

磷酸银
/ 光催化
/ Z型体系
/ 应用
/ 机理

English

Recent progress in Ag₃PO₄-based all-solid-state Z-scheme photocatalytic systems

Ming Ge ^a,b, ,
Zhenlu Li ^a,

a College of Chemical Engineering, North China University of Science and Technology, Tangshan 063210, Hebei, China;
b Hebei Key Laboratory of Photocatalytic and Electrocatalytic Materials for Environment, Tangshan 063210, Hebei, China
Received Date: 30 June 2017
Revised Date: 18 August 2017
Fund Project:
This work was supported by the Youth Foundation of Hebei Education Department (QN2017115), and the National Natural Science Foundation of China (51504079).

Abstract: Heterogeneous semiconductor photocatalysis is a promising green technology solution to energy and environmental problems. Traditional photocatalyst TiO₂, with a wide band gap of 3.2 eV, can only be excited by UV light and utilizes less than 4% of solar energy. Silver phosphate (Ag₃PO₄) is among the most active visible-light-driven photocatalysts reported. Unfortunately, unwanted pho-tocorrosion is the main obstacle to the practical application of Ag₃PO₄. Much effort has been made in recent years to address this issue and further enhance the photocatalytic performance of Ag₃PO₄. The construction of Z-scheme photocatalytic systems that mimic natural photosynthesis is a prom-ising strategy to improve the photocatalytic activity and stability of Ag₃PO₄. This brief review con-cisely summarizes and highlights recent research progress in Ag₃PO₄-based all-solid-state Z-scheme photocatalytic systems with or without a solid-state electron mediator, focusing on their construc-tion, application, and reaction mechanism. Furthermore, the challenges and future prospects of Ag₃PO₄-based Z-scheme photocatalytic systems are discussed.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

基于Ag₃PO₄的全固态Z型光催化体系研究进展

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