Design Principles for Maximizing Hole Utilization of Semiconductor Quantum Wires toward Efficient Photocatalysis

Zhang, Chong1; Shao, Zhen-Chao1; Zhang, Xiao-Long1; Liu, Guo-Qiang1; Zhang, Yu-Zhuo1; Wu, Liang1; Liu, Cheng-Yuan2; Pan, Yang2; Su, Fu-Hai3; Gao, Min-Rui1; Li, Yi1; Yu, Shu-Hong1,4

2023-07-01

10.1002/anie.202305571

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Maximizing hole-transfer kinetics-usually a rate-determining step in semiconductor-based artificial photosynthesis-is pivotal for simultaneously enabling high-efficiency solar hydrogen production and hole utilization. However, this remains elusive yet as efforts are largely focused on optimizing the electron-involved half-reactions only by empirically employing sacrificial electron donors (SEDs) to consume the wasted holes. Using high-quality ZnSe quantum wires as models, we show that how hole-transfer processes in different SEDs affect their photocatalytic performances. We found that larger driving forces of SEDs monotonically enhance hole-transfer rates and photocatalytic performances by almost three orders of magnitude, a result conforming well with the Auger-assisted hole-transfer model in quantum-confined systems. Intriguingly, further loading Pt cocatalyts can yield either an Auger-assisted model or a Marcus inverted region for electron transfer, depending on the competing hole-transfer kinetics in SEDs.

Hole Transfer Kinetics Photocatalysis Quantum Confinement Sacrificial Electron Donors

SCI ; EI

英语

NI论文

通讯

National Key Research and Development Program of China["2018YFE0202201","2021YFA0715700"] ; National Natural Science Foundation of China["U1932213","22271265","22101270"] ; University Synergy Innovation Program of Anhui Province[GXXT-2019-028] ; Natural Science Foundation Youth Project of Anhui Province[2108085QB74] ; Key Cooperation Project of Chinese Academy of Engineering[2021-4/2021-6] ; USTC Research Funds of the Double First-Class Initiative[YD9990002013] ; Fundamental Research Funds for the Central Universities[WK2060000031]

Chemistry

Chemistry, Multidisciplinary

WOS:001031568500001

WILEY-V C H VERLAG GMBH

20232814383083

Augers ; Electrons ; Hydrogen production ; II-VI semiconductors ; Kinetics ; Nanowires ; Selenium compounds ; Semiconductor quantum wells ; Solar power generation ; Zinc compounds

Mine and Quarry Equipment:502.2 ; Gas Fuels:522 ; Solar Power:615.2 ; Fluid Flow, General:631.1 ; Semiconducting Materials:712.1 ; Semiconductor Devices and Integrated Circuits:714.2 ; Nanotechnology:761 ; Classical Physics; Quantum Theory; Relativity:931 ; Solid State Physics:933

CHEMISTRY

Web of Science

1.Univ Sci & Technol China, Inst Biomimet Mat & Chem, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem,Div Nanomat & Chem,New Cornerstone Sci L, Hefei 230026, Peoples R China
2.Univ Sci & Technol China, Synchrotron Radiat Lab, Hefei 230029, Peoples R China
3.Chinese Acad Sci, Inst Solid State Phys, Key Lab Mat Phys, HFIPS, Hefei 230031, Peoples R China
4.Southern Univ Sci & Technol, Inst Innovat Mat I2 M, Dept Mat Sci & Engn, Dept Chem, Shenzhen 518055, Peoples R China

Zhang, Chong,Shao, Zhen-Chao,Zhang, Xiao-Long,et al. Design Principles for Maximizing Hole Utilization of Semiconductor Quantum Wires toward Efficient Photocatalysis[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023,62(33).

Zhang, Chong.,Shao, Zhen-Chao.,Zhang, Xiao-Long.,Liu, Guo-Qiang.,Zhang, Yu-Zhuo.,...&Yu, Shu-Hong.(2023).Design Principles for Maximizing Hole Utilization of Semiconductor Quantum Wires toward Efficient Photocatalysis.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,62(33).

Zhang, Chong,et al."Design Principles for Maximizing Hole Utilization of Semiconductor Quantum Wires toward Efficient Photocatalysis".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62.33(2023).