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 Material Science&Engineering,Northeastern University,Shenyang 110819,China [4]Institute of Technology for Carbon Neutrality,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China
出 处:《Science Bulletin》2022年第23期2420-2427,M0004,共9页科学通报(英文版)
基 金:the National Key Research and Development Program of China (2021YFA1500800);National Natural Science Foundation of China (51825204, 52072377, and 52188101);Youth Innovation Promotion Association of the Chinese Academy of Sciences (2020192);International Partnership Program of the Chinese Academy of Sciences (174321KYSB20200005);Natural Science Foundation of Liaoning Province (2021-MS-014) for the financial support。
摘 要:Semiconductor heterostructures mediated by electrical conductors are very promising for Z-scheme photocatalytic water splitting.In contrast to conventional particulate heterostructures,alternate TiO_(2)and Cu_(2)O film stripes patterned parallel on a fluorine-doped tin oxide(FTO) conductive substrate was fabricated as a model film photocatalyst to study the characteristics of the photogenerated charge transfer process.The Z-scheme transfer process with an effective transport distance of up to 5 μm occurs only in regions distant from the TiO_(2)/Cu_(2)O strip edges through the FTO substrate from the bottom.In contrast,the transfer of charge around their contact regions follows the conventional transfer process through the TiO_(2)/Cu_(2)O strip interface.These results indicate that the Z-scheme transfer process occurring in such a large region dominates the charge transfer processes in the TiO_(2)/FTO/Cu_(2)O pattern film heterostructure.Importantly,unlike the single component film,which is inactive for photocatalytic overall water splitting,the modified TiO_(2)/Cu_(2)O pattern film can induce photocatalytic overall water splitting at a stoichiometric H_(2)/O_(2) ratio close to 2:1.These findings have significant implications in designing efficient heterostructures by employing a Z-scheme charge transfer process.基于导电媒介所构建的具有Z型电荷转移机制的半导体异质结构在实现高效太阳能驱动光催化全分解水方面极具潜力.不同于传统颗粒型异质结构,本文采用具有高可控性的微纳集成手段,在氟掺杂氧化锡(FTO)导电基底上集成了TiO_(2)、Cu_(2)O交替条带平行排列的图案化薄膜光催化材料,该异质结构中形成了TiO_(2)/Cu_(2)O和TiO_(2)/FTO/Cu_(2)O两种接触界面.通过光化学沉积示踪方法研究了光生电荷的跨界面转移机制,结果表明TiO_(2)/Cu_(2)O直接接触界面附近的光生电荷遵循传统电荷转移机制,而远离TiO_(2)/Cu_(2)O接触边界区域的条带中光生电荷则通过底部的FTO导电基体实现Z型电荷转移,其有效作用距离长达约5μm,是该体系中的主要电荷转移机制.该TiO_(2)/Cu_(2)O图案化薄膜展现出全光谱下光催化全解水的能力,所产生的H_(2)/O_(2)化学计量比接近2:1.此研究为设计具有高效Z型电荷转移过程的异质结构光催化材料提供了重要的借鉴作用.
关 键 词:PHOTOCATALYST Pattern film Heterostructure Z-scheme Water splitting
分 类 号:TQ116.2[化学工程—无机化工] TQ426[一般工业技术—材料科学与工程] TB383.2
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