期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 32, 页码 17601-17607出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104754
关键词
oxygen vacancies; photocharging; discharging; p-n heterojunctions; solar water splitting; tungsten
资金
- National Natural Science Foundations of China [51802320, 21965024]
- 111 project [D20033]
- Central Government Guiding Special Funds for the Development of Local Science and Technology [2020ZY0012]
- Natural Science Foundation of Inner Mongolia Autonomous Region of China [2020JQ01]
- Inner Mongolia University [21300-5195102, 10000-21311201/006]
- opening project of Key Laboratory of Materials Processing and Mold from Zhengzhou University
A photocharge/discharge strategy significantly improves the performance of the WO3 photoelectrode while maintaining its stability. Additionally, the study shows that the photocharged WO3/CuO heterojunction structure enables effective photoinduced electron transfer.
A photocharge/discharge strategy is proposed to initiate the WO3 photoelectrode and suppress the main charge recombination, which remarkably improves the photoelectrochemical (PEC) performance. The photocharged WO3 surrounded by a 8-10 nm overlayer and oxygen vacancies could be operated more than 25 cycles with 50 h durability without significant decay on PEC activity. A photocharged WO3/CuO photoanode exhibits an outstanding photocurrent of 3.2 mA cm(-2) at 1.23 V-RHE with a low onset potential of 0.6 V-RHE, which is one of the best performances of p-n heterojunction structure. Using nonadiabatic molecular dynamics combined with time-domain DFT, we clarify the prolonged charge carrier lifetime of photocharged WO3, as well as how electronic systems of photocharged WO3/CuO semiconductors enable the effective photoinduced electrons transfer from WO3 into CuO. This work provides a feasible route to address excessive defects existed in photoelectrodes without causing extra recombination.
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