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用于增强光催化全水分解的 SrTiO 上的协同表面氧缺陷和体相 Ti 缺陷工程

Synergistic surface oxygen defect and bulk Ti defect engineering on SrTiO for enhancing photocatalytic overall water splitting.

作者信息

Su Zhiyuan, Fang Fan, Li Xue, Han Wenjun, Liu Xianglei, Chang Kun

机构信息

Centre for Hydrogenergy, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, PR China.

College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.

出版信息

J Colloid Interface Sci. 2022 Nov 15;626:662-673. doi: 10.1016/j.jcis.2022.06.109. Epub 2022 Jun 25.

Abstract

SrTiO as a photocatalytic overall water splitting material has received extensive attention in recent years, while effectively suppressing Ti is the key to enhancing the photocatalytic performance. Herein, a polymerizable complexation method is employed to enable Al uniformly enter into SrTiO lattice for reducing Ti, and substituting Ti with the formation of oxygen vacancy. Thus, the photogenerated carrier transport is promoted, and the resulting appropriate surface oxygen vacancy is also conducive to the adsorption of water molecules and OH*. The optimized 2% Al-doped SrTiO possesses a lower Ti concentration, compared with the same sample prepared by the solid-phase griding method. Consequently, 2% Al-STO sample deposited co-catalysts achieves the highest activity and durability with the H and O evolution rates of 1.256 mmol·h and 0.692 mmol·h (0.04 g catalyst), respectively, corresponding to the AQE value of 55.46% at 365 nm. The characterizations and DFT calculation results reveal that the uniform Al doping promotes the increase in the surface oxygen vacancy, which is beneficial for accelerating the reduction reaction and facilitating carrier separation and migration, therefore enhancing the overall water splitting reaction.

摘要

近年来,SrTiO作为一种光催化全分解水材料受到了广泛关注,而有效抑制Ti是提高光催化性能的关键。在此,采用可聚合络合法使Al均匀进入SrTiO晶格以还原Ti,并通过形成氧空位来替代Ti。因此,促进了光生载流子的传输,并且所产生的适当表面氧空位也有利于水分子和OH*的吸附。与通过固相研磨法制备的相同样品相比,优化后的2%Al掺杂SrTiO具有更低的Ti浓度。因此,负载了助催化剂的2%Al-STO样品实现了最高的活性和耐久性,析氢和析氧速率分别为1.256 mmol·h和0.692 mmol·h(0.04 g催化剂),在365 nm处对应的AQE值为55.46%。表征和DFT计算结果表明,均匀的Al掺杂促进了表面氧空位的增加,这有利于加速还原反应并促进载流子的分离和迁移,从而增强全分解水反应。

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