钒酸盐光催化剂晶面及表界面调控增强光催化分解水性能研究

In this proposal, efficient visible-light responsive vanadate polyhedrons photocatalysts will be fabricated via its surface atomic arrangement to improve separation and migration of photo-excited carriers. Following work will be studied: (1) vanadate polyhedrons will be synthesized and stabilized by solvothermal method or ionic absorption, while the correlation between crystal facets and photocatalytic water splitting effect will be investigated via surface absorption/desorption of water molecule and seperation/migration photo-excited carriers ; (2) the interaction between surface properties of atomic arrangement and photocatalytic activity will be studied by varying surface atom structure, incoordinated atom, atomic step and so on; (3) reaction mechanism of photocatalytic water splitting on vanadate polyhedrons will be analyzed by studying the effect of crystal facets exposed ratio, surface atomic arrangement. In summary, vanadate polyhedrons photocatalysts will be studied via surface atomic arrangement and the efficient crystal facets will be confirmed by photocatalytic water splitting, which will be beneficial to the modulation and selection of crystal facets in photocatalysis.

本项目从晶面原子结构设计出发，以空间光生载流子有效分离与迁移为目标制备出可见光响应、高效光解水活性的钒酸盐多面体光催化剂。拟进行如下研究：(1)采用溶剂热、离子吸附法设计和制备出稳定的钒酸盐多面体光催化剂，结合表界面水分子吸附脱附性能和光生载流子行为研究暴露晶面与光解水之间的构-效关系；(2)分析晶面的原子结构、非对称原子、原子台阶等探明表面物理化学性质与光催化性能影响的规律；(3)综合分析钒酸盐光解水催化剂晶面暴露比例、晶面原子结构、氧化还原之间的相互关系，探究光解水氧化还原反应机理。本项目从晶面原子结构角度设计和制备钒酸盐光催化剂，通过晶面与光解水性能的构-效关系确定高效晶面，对半导体晶面的调控和筛选具有重要的指导意义。

中文摘要：在本项目的资助下，研究工作主要集中在以下三方面：1）无机半导体催化剂的可控制备，完成了钒酸盐、钼酸盐等一系列三元光催化剂的可控合成，并总结了溶剂、温度、形貌导向剂等对结构的影响；2）三元光催化剂晶面原子排布，分析原子排布、态密度、能带结构对催化剂物化性质的影响，提取微观结构-宏观性质间的关系；3）研究三元钒酸盐、钼酸盐的结构与光催化性能关系，结合催化剂的能带结构、光捕获范围、载流子迁移和传输，反应前驱体的性质等，分析催化剂微观结构与光催化性能间的构-效关系。本项目从本质原因出发，探究了钒酸盐晶面与催化性能的构效关系，为高效光催化剂的可控制备提供借鉴意义。