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Photo‐driven Oxygen Vacancies Extends Charge Carrier Lifetime for Efficient Solar Water Splitting
Author(s) -
Sun Mao,
Gao RuiTing,
He Jinlu,
Liu Xianhu,
Nakajima Tomohiko,
Zhang Xueyuan,
Wang Lei
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202104754
Subject(s) - overlayer , photocurrent , charge carrier , materials science , heterojunction , semiconductor , water splitting , recombination , charge (physics) , optoelectronics , oxygen , electron , carrier lifetime , chemical physics , atomic physics , photocatalysis , chemistry , physics , silicon , biochemistry , organic chemistry , quantum mechanics , gene , catalysis
A photocharge/discharge strategy is proposed to initiate the WO 3 photoelectrode and suppress the main charge recombination, which remarkably improves the photoelectrochemical (PEC) performance. The photocharged WO 3 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 WO 3 /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 WO 3 , as well as how electronic systems of photocharged WO 3 /CuO semiconductors enable the effective photoinduced electrons transfer from WO 3 into CuO. This work provides a feasible route to address excessive defects existed in photoelectrodes without causing extra recombination.