具有d10-d10金属间相互作用的银铋三元氧化物的光催化氧化性能研究

项目名称： 具有d10-d10金属间相互作用的银铋三元氧化物的光催化氧化性能研究

项目编号： No.21501177

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 数理科学和化学

项目作者： 马祖驹

作者单位： 安徽工业大学

项目金额： 20万元

中文摘要： 光催化氧化技术不仅应用于光分解水，还用于治理环境污染。发展一种稳定、无毒且具有高活性的可见光光催化剂是该技术走向实用化的关键。最新研究表明，金属间d10-d10相互作用是引起Ag3PO4等半导体光催化剂高活性的一个重要原因，对此进行更深入的研究对发现高活性光催化剂具有重要意义。本项目拟结合密度泛函理论方法和实验手段，从体相到表面对一系列包含多种金属间相互作用（d10-d10、d10-d10s2等）的Ag-Bi-O化合物及Ag-Bi1-xMx-O固溶体的能带结构和光催化氧化性能进行系统研究，探索它们在光催化氧化水及光降解有机污染物中的潜在应用价值。考察金属间d10-d10相互作用对体系能隙、氧化还原势、载流子迁移和分离、表面电子结构及表面水氧化反应能垒等光催化性能参数的影响规律，探索银基氧化物光催化活性的结构根源并提出优化机制，为发展新型金属氧化物光催化剂提供理论依据。

中文关键词： 第一性原理；能带调控；光催化剂；银基氧化物；电子结构

英文摘要： Photocatalysis oxidation technology is not only used for photocatalytic water splitting, but also for remedying environmental pollution. The practicality of this technology requires a stable, non-toxic and high visible-light active photocatalyst. The latest researches show that the superior photocatalytic activities in some siliver-based oxides, such as Ag3PO4, are correlated with the spatial proximity between Ag ions stabilized by d10-d10 interaction. It is of great importance to make an intensive study of this phenomenon in hope of finding more highly active photocatalysts. In this program, we will investigate the electronic properties and photocatalytic oxidation activity of Ag-Bi-O ternary oxides and Ag-Bi1-xMx-O solid solutions based on their bulk cells and surfaces by using both the density functional methods and experimental methods. These oxides present many types of metal-metal interaction, such as d10-d10s0, d10-d10s2, etc. The potential applications of Ag-Bi-O compounds and Ag-Bi1-xMx-O solid solutions in photocatalytic water splitting and degradation of dye wastewater will be investigated. The effect of the d10-d10 interactions between metals on the photocatalytic properties including the energy band gap, the redox potentials, the mobility and recombination rate of photo-induced carriers, the electronic structure of surface and the energy barrier of photocatalytic water oxidation reaction will be revealed. The structural origin of the photocatalytic oxidation activity and the corresponding optimization mechanism will be investigated. The study will provide theoretical basis towards developing the new visible-light photocatalysts from metal oxides.

英文关键词： First principles;Band engineering;Photocatalyst;Siliver-based oxides;Electronic structure