可回收型各向同性热解石墨导电基底促进光电化学水分解  

Boosting photoelectrochemical water splitting with recyclable isotropic pyrolytic graphite conductive substrates

作　　者：徐伟 甄超 邱建航 杜宇飞 白朔 成会明 刘岗 Wei Xu;Chao Zhen;Jianhang Qiu;Yufei Du;Shuo Bai;Hui-Ming Cheng;Gang Liu(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;Shi-Changxu Innovation Center for Advanced Materials,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China;Institute of Technology for Carbon Neutrality,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China)

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]Shi-Changxu Innovation Center for Advanced Materials,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China [4]Institute of Technology for Carbon Neutrality,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China

出　　处：《Science China Materials》2023年第12期4663-4668,共6页中国科学（材料科学）（英文版）

基　　金：financially supported by the National Key R&D Program of China (2021YFA1500800);the National Natural Science Foundation of China (51825204, 52072377, and 52188101);the Youth Innovation Promotion Association of the Chinese Academy of Sciences (2020192);the Natural Science Foundation of Liaoning Province (2021MS-014);the financial support from the New Cornerstone Science Foundation through the XPLORER PRIZE

摘　　要：导电基底发挥着收集和传输光生电荷的关键作用,是光电化学(PEC)水分解用光电极不可或缺的重要组成部分,但构建高效光电极鲜受关注.本工作中,基于各向同性热解石墨(IPG)高电导率和高功函的特性,我们开发了各向同性热解石墨(IPG)作为一种导电基底来构建高性能光电极.相比于氟掺杂的二氧化锡(FTO)和金属箔片等广泛使用的导电基底,该光电极能与Cu_(2)O形成欧姆接触,因此所得IPG/Cu_(2)O光电阴极呈现出比FTO/Cu_(2)O光阴极高60%的光电流密度.IPG基底上经过高温氮化所得的Ta_(3)N5薄膜(IPG/Ta_(3)N_(5))可以获得与Ta箔负载的Ta_(3)N_(5)光阳极相媲美的PEC性能.此外,Ta箔由于在氮化过程中会出现严重氢脆问题而不能循环使用,而IPG基底则可以循环用于光电极的制备,且能生长出具有相同PEC性能的半导体薄膜.这项工作为通过碳基导电基底构建用于PEC水分解的高效光电极提供了一种有吸引力的可替代选择.The conductive substrates as indispensable component of photoelectrodes play a critical role in collecting photogenerated charges for efficient photoelectrochemical(PEC)water splitting but have been less concerned in constructing photoelectrodes.Here,we exploited the isotropic pyrolytic graphite(IPG)as a kind of recyclable conductive substrates for the construction of high-performance photoelectrodes.Compared with widely used conductive substrates such as fluorine-doped tin oxide(FTO)and metal foils,IPG reveals the merits of high electrical conductivity,large work function,and good resistance to high-temperature treatment and embrittlement in reductive atmospheres for superior photoelectrodes.The resulting IPG/Cu_(2)O photocathode can deliver a higher photocurrent density by over 60%than the reference FTO/Cu_(2)O photocathode,benefiting from the large work function of IPG that facilitates the formation of Ohmic contact with Cu_(2)O.The high-temperature nitrided Ta3N5 photoactive film on the IPG substrate(IPG/Ta_(3)N_(5))can display PEC performance superior to that of the Ta foil-supported Ta_(3)N_(5)photoanode.Moreover,in contrast to the Ta foils,which exhibit typically unrecyclable characteristics due to serious hydrogen embrittlement in nitridation,the IPG substrate could be recycled to grow semiconductor films with identical PEC performance.This work offers an alternative and attractive choice of constructing efficient photoelectrodes via carbon-based conductive substrates for PEC water splitting.

关 键 词：isotropic pyrolytic graphite PHOTOELECTROCHEMICAL recycleable ohmic contact conductive substrate 

分 类 号：O646[理学—物理化学] TQ127.11[理学—化学]