摘要
In_(2)O_(3)作为一种n型半导体,被认为是合成氨基酸最有前途的光催化剂之一,然而In_(2)O_(3)自身在光生电荷动力学方面存在不足.我们通过一步溶剂热和煅烧法合成了具有多孔棒状结构的Mo原子掺杂In_(2)O_(3)(Mo-In_(2)O_(3)).在可见光照射下,将Mo-In_(2)O_(3)用于乳酸转化为丙氨酸的反应,实现了81%的转化率和91%的选择性.光谱技术和密度泛函理论计算表明, Mo原子引入了略低于In_(2)O_(3)导带的缺陷能级,改善了光生电子-空穴对的分离效率.此外, In_(2)O_(3)表面上的Mo原子形成新的吸附和反应活性中心,可显著提高催化反应速率.本工作为开发过渡金属单原子修饰的半导体光催化剂应用于氨基酸生产提供了理论基础.
As an n-type semiconductor, In_(2)O_(3)is considered a promising photocatalyst for producing amino acids using biomass derivatives as precursors. However, similar to other intrinsic semiconductors, In_(2)O_(3)suffers from poor charge dynamics. Herein, we show the synthesis of Mo-doped In_(2)O_(3)(Mo-In_(2)O_(3)) with a porous rod-shaped structure through a onestep solvothermal reaction followed by calcination. Under visible-light irradiation, Mo-In_(2)O_(3)achieves a high conversion rate of 81% for the reaction that transforms lactic acid into alanine with a selectivity of 91%. Spectroscopic techniques and density functional theory calculations reveal that Mo doping introduces defect states slightly below the conduction band of In_(2)O_(3), which improves the separation of photogenerated electron-hole pairs. In addition, Mo atoms on the surface form extra adsorption and reaction centers that greatly enhance the reaction rate. This work provides insights into the development of transition metal-doped semiconductor photocatalysts to produce amino acids.
作者
郑芒
李琪
刘明洋
刘佳男
赵陈
肖旭东
王洪丽
周靖
张莉平
蒋保江
Mang Zheng;Qi Li;Mingyang Liu;Jianan Liu;Chen Zhao;Xudong Xiao;Hongli Wang;Jing Zhou;Liping Zhang;Baojiang Jiang(School of Chemistry and Materials Science,Heilongjiang University,Harbin 150080,China;College of Material Science and Chemical Engineering,Harbin Engineering University,Harbin 150001,China;Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen 518055,China;Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201800,China)
基金
supported by the National Natural Science Foundation of China (21771061)
the Outstanding Youth Fund of Heilongjiang Province (JQ 2020B002)
the support of the SUSTech Presidential Postdoctoral Fellowship。
