摘要
目前,人们面临着日益严重的能源与环境危机.氢气是一种清洁能源,而通过光解水制氢成为解决上述问题的有效途径.光吸收及电子空穴分离是决定光解水能量转化效率的关键因素,对于它们的研究有助于人们开发高效的光解水制氢材料.二维材料由于具有较大的比表面积、载流子迁移路程短、优异的光学性质等特性,引起了人们的广泛关注.本文从理论上介绍了二维光解水制氢材料的最新进展.其中包括:通过筛选、设计及调控的方法寻找新的二维光解水材料;通过分子设计和化学改性方法增强二维材料的光吸收性能;通过构建二维范德华异质结促进光生电子和空穴的分离;通过引入内禀电场的手段同时增强光吸收及光生电子和空穴的分离.另外,本文展望了二维光解水制氢材料理论研究所面临的机遇和挑战.
Currently,the energy and environment associated problems become more and more serious.Hydrogen is a kind of clean and renewable resource.Hydrogen generation through photocatalytic water splitting is a feasible and efficient route to resolve these problems.In general,the photocatalytic water splitting process is composed of three pivotal steps:Light harvest,carrier separation and transportation,and hydrogen evolution reaction(HER)as well as oxygen evolution reaction(OER).Improving the efficiencies of these three steps are keys to enhance the solar-to-hydrogen(STH)efficiency,which stimulates the development of high-performance photocatalysts.Typically,for two-dimensional(2D)materials,the photogenerated electrons and holes produce directly from the surfaces of 2D materials with atomic thickness.In addition,compared with their bulk counterparts,2D materials with an extremely large specific surface area,rather high carrier mobility,and controllable interfaces offer a large number of advantages for the photocatalysts exploration.Thus,search and design of 2D photocatalysts for water splitting has been a hot topic.Density functional theory(DFT)based first-principles calculations is a powerful tool for materials design and has been widely used in exploring 2D photocatalysts for water splitting.Here,recent advances in the design of 2D materials for photocatalytic water splitting are presented from a theoretical perspective.In the initial stage,a great of new 2D photocatalysts for water splitting are expected to be discovered.Mechanical and chemical assisted exfoliation of layered materials is straightforward approaches to get access to single-layer and few-layer2D materials.By using DFTcalculations,many potential 2D photocatalysts are screened out for water splitting.In addition,molecular designing and chemical regulating are alternative approaches for exploring new 2D photocatalysts for water splitting.The light harvest is the initial process of photocatalytic water splitting,and increasing the light adsorption is one of
作者
付岑峰
杨金龙
Cenfeng Fu;Jinlong Yang(Hefei National Laboratory for Physical Sciences at the Microscale,Department of Chemical Physics,Synergetic Innovation Center of Quantum Information&Quantum Physics,University of Science and Technology of China,Hefei 230026,China)
出处
《科学通报》
EI
CAS
CSCD
北大核心
2021年第6期591-605,共15页
Chinese Science Bulletin
基金
国家重点研发计划(2016YFA0200604)
国家自然科学基金(21688102)
安徽量子通信与量子计算机重大项目(AHY090400)资助。
关键词
第一性原理计算
二维材料
光解水
能带调控
first-principles calculations
two-dimensional materials
photocatalytic water splitting
band engineering
