Selectively constructing sandwich-like heterostructure of CdS/PbTiO_(3)/TiO_(2)to improve visible-light photocatalytic H_(2)evolution  

选择性构建“三明治”型CdS/PbTiO_(3)/TiO_(2)异质结构提升可见光光催化产氢活性

作　　者：Gedeng Wan Yongqiang Yang Huaze Zhu Chao Zhen Xiaoxiang Xu Lianzhou Wang Gang Liu 万格灯;杨勇强;朱华泽;甄超;徐晓翔;王连洲;刘岗(Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China;School of Materials Science and Engineering,University of Science and Technology of China,Shenyang 110016,China;School of Chemical Science and Engineering,Tongji University,Shanghai 200060,China;Nanomaterials Centre,School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology,The University of Queensland,QLD 4072,Australia)

机构地区：[1]Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China [2]School of Materials Science and Engineering,University of Science and Technology of China,Shenyang 110016,China [3]School of Chemical Science and Engineering,Tongji University,Shanghai 200060,China [4]Nanomaterials Centre,School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology,The University of Queensland,QLD 4072,Australia

出　　处：《Science China Materials》2022年第12期3428-3434,共7页中国科学（材料科学（英文版）

基　　金：the National Key R&D Program of China(2021YFA1500800);the National Natural Science Foundation of China(51825204,52120105003,and 52072379).

摘　　要：Fast migration and efficient spatial separation of photogenerated charges in photocatalytic materials are indispensable to efficient solar water splitting reactions.Here,we construct a three-phase heterostructure of CdS/PbTiO_(3)/TiO_(2)by selectively depositing CdS and TiO_(2)at oppositely poled crystal facets of PbTiO_(3)using single-domain ferroelectric PbTiO_(3).The heterostructure has matching band edge alignments and strong interfacial connections at different moieties.The heterostructure combines the interfacial electrical and ferroelectric fields because of their peculiar microstructures,which provide a strong driving force throughout the whole bulk to separate photogenerated charges.Almost two orders of magnitude improvement of visible-light-driven photocatalytic H_(2) production has been realized in CdS/PbTiO_(3)/TiO_(2)compared with bare PbTiO_(3)/TiO_(2),showing the efficiency of charge separation in the heterostructure.The idea of combining ferroelectrics with potential light capture semiconductor provides a paradigm to accurately design charge migration pathways,bringing a step closer to efficient solar water splitting.光生电荷的快速迁移和高效分离是实现高效太阳能分解水反应的必要条件.本文中,我们通过铁电单畴PbTiO_(3)晶体的不同极性晶面对阴阳离子的选择性吸附,在其正负极性面上分别选择性生长了TiO_(2)和CdS,构建出了“三明治”型CdS/PbTiO_(3)/TiO_(2)异质结构,且CdS和TiO_(2)均与PbTiO_(3)晶体具有高质量的界面接触.在该“三明治”型结构中通过单畴铁电场与界面电场的结合,CdS、PbTiO_(3)和TiO_(2)三种材料的能带实现了有序级联,为整个体系提供了促进光生电荷迁移和分离的强驱动力.用于可见光催化产氢反应中,CdS/PbTiO_(3)/TiO_(2)的活性较PbTiO_(3)/TiO_(2)提升了两个数量级,显示了“三明治”型结构的高电荷分离特性.本工作中所展示的利用铁电场实现不同半导体能带结构有序级联的策略,为光电荷迁移与分离路径的合理设计提供了一种新思路.

关 键 词：photocatalysis FERROELECTRIC PBTIO3 water splitting HETEROSTRUCTURE 

分 类 号：TQ116.2[化学工程—无机化工] O643.36[理学—物理化学] O644.1[理学—化学]