二维铟-VA族半导体:具有本征电场用于分解水的高效光催化剂  

2D indium-VA semiconductors:Promising photocatalysts with intrinsic electric fields for water splitting

作　　者：刘晓庆 凌发令 Xiaoqing Liu;Faling Ling(School of Science,Chongqing University of Posts and Telecommunications,Chongqing 400065,China;College of Optoelectronic Engineering,Chongqing University,Chongqing 400044,China;Key Laboratory of Optoelectronic Information Sensing and Transmission Technology,Chongqing University of Posts and Telecommunications,Chongqing 400065,China)

机构地区：[1]School of Science,Chongqing University of Posts and Telecommunications,Chongqing 400065,China [2]College of Optoelectronic Engineering,Chongqing University,Chongqing 400044,China [3]Key Laboratory of Optoelectronic Information Sensing and Transmission Technology,Chongqing University of Posts and Telecommunications,Chongqing 400065,China

出　　处：《Science China Materials》2023年第7期2759-2767,共9页中国科学（材料科学（英文版）

基　　金：supported by the Scientific and Technological Research Program of Chongqing Municipal Education Commission(KJQN202000629);the Natural Science Foundation of Chongqing(cstc2020jcyj-msxmX0692);the financial support from China Scholarship Council(202106050115)。

摘　　要：近年来,含有本征电场的二维半导体材料因拥有抑制光生载流子复合的潜在能力而受到了光催化领域研究人员的广泛关注.在本文中,我们采用第一性原理计算方法,报道了一类具有本征极性的新型二维半导体材料一单层铟-VA族化合物(ML-InXs;X=P、As和Sb),并探究了它们作为光催化剂分解水的可能.我们系统地研究了ML-InXs的几何结构、电子结构和光学性质,发现它们具有优异的结构稳定性、合适的带隙和带边位置、出色的载流子迁移率和较广的光吸收范围,因此可以成为水分解反应的优秀光催化剂.更重要的是,在ML-InXs中由本征偶极矩产生的电场可抑制光生电子-空穴对复合,大大提高了光催化反应过程中的能量转换效率.此外,我们发现应变工程可以有效地调节ML-InXs的带隙和光吸收,并显著提高它们分解水时的太阳能转化效率.我们的研究进一步加深了人们对具有本征电场的二维光催化剂的理解,并可为未来设计出具有优异性能的水分解或其他重要化学反应的光催化剂提供理论指导.Exploration of two-dimensional(2D)semiconductors with intrinsic electric fields for photocatalytic applications has recently attracted great attention due to their prospective ability to inhibit the recombination of photogenerated carriers.Herein,employing first-principles calculations,we report a new group of 2D semiconductors,monolayer indium-VA(ML-InXs;X=P,As,and Sb),with intrinsic dipole as potential photocatalysts for water splitting.We systematically investigated the geometry,electronics and optics of ML-InXs,and identified their excellent structural stability,suitable band gaps,appropriate band edge positions,outstanding carrier transport and wide range of light absorption,which make them excellent photocatalysts for water splitting.More importantly,the electric field induced by the intrinsic dipole in ML-InXs would suppress the recombination of photogenerated electron-hole pairs,greatly enhancing the energy conversion efficiency during the photocatalytic reaction.In addition,we find that strain engineering can effectively tune the band gap and light absorption of ML-InXs and significantly enhance their solar-to-hydrogen efficiency for water splitting.Our results provide fundamental insight into the 2D photocatalysts with an intrinsic electric field and shed light on future design and modification of superior photocatalysts for water splitting and other important chemical reactions.

关 键 词：indium-VA semiconductor PHOTOCATALYST intrinsic electric field water splitting strain engineering 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学]