Wang Xuehua, Wang Xianghu, Huang Jianfeng, Li Shaoxiang, Meng Alan, Li Zhenjiang
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao, Shandong, P. R. China.
Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE. College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, Shandong, P. R. China.
Nat Commun. 2021 Jul 5;12(1):4112. doi: 10.1038/s41467-021-24511-z.
Construction of Z-scheme heterostructure is of great significance for realizing efficient photocatalytic water splitting. However, the conscious modulation of Z-scheme charge transfer is still a great challenge. Herein, interfacial Mo-S bond and internal electric field modulated Z-scheme heterostructure composed by sulfur vacancies-rich ZnInS and MoSe was rationally fabricated for efficient photocatalytic hydrogen evolution. Systematic investigations reveal that Mo-S bond and internal electric field induce the Z-scheme charge transfer mechanism as confirmed by the surface photovoltage spectra, DMPO spin-trapping electron paramagnetic resonance spectra and density functional theory calculations. Under the intense synergy among the Mo-S bond, internal electric field and S-vacancies, the optimized photocatalyst exhibits high hydrogen evolution rate of 63.21 mmol∙g·h with an apparent quantum yield of 76.48% at 420 nm monochromatic light, which is about 18.8-fold of the pristine ZIS. This work affords a useful inspiration on consciously modulating Z-scheme charge transfer by atomic-level interface control and internal electric field to signally promote the photocatalytic performance.
构建Z型异质结构对于实现高效光催化水分解具有重要意义。然而，有意识地调控Z型电荷转移仍然是一个巨大的挑战。在此，通过富含硫空位的ZnInS和MoSe合理构建了界面Mo-S键和内电场调制的Z型异质结构，用于高效光催化析氢。系统研究表明，表面光电压谱、DMPO自旋捕获电子顺磁共振谱和密度泛函理论计算证实，Mo-S键和内电场诱导了Z型电荷转移机制。在Mo-S键、内电场和S空位之间的强烈协同作用下，优化后的光催化剂在420 nm单色光下表现出63.21 mmol∙g·h的高光催化析氢速率和76.48%的表观量子产率，约为原始ZIS的18.8倍。这项工作为通过原子级界面控制和内电场有意识地调控Z型电荷转移以显著提高光催化性能提供了有益的启示。
