Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 32, Pages 12499-12508Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00802
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Funding
- National Natural Science Foundation of China [21902157, 22088102, 22090033]
- National Postdoctoral Program for Innovative Talent [BX20180296]
- China Postdoctoral Science Foundation [2018M641720]
- Natural Science Foundation of Liaoning Province [2019-BS-239]
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB17000000]
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This study achieved efficient unassisted overall water splitting by using a photoelectrochemical platform with multimediator modulation, increasing solar energy conversion efficiency. By assembling an integrated system composed of inorganic oxide-based photoanode and organic polymer-based photocathode, the efficiency of solar-to-hydrogen conversion was successfully improved.
Photoelectrochemical overall water splitting has been considered as a promising approach for producing chemical energy from solar energy. Although many photoelectrochemical cells have been developed for overall water splitting by coupling two semiconductor photoelectrodes, inefficient charge transfer between the light-harvesters and electron acceptor/donor severely restricts the solar energy conversion efficiency. Inspired by natural photosynthesis, we assembled a photoelectrochemical platform with multimediator modulation to achieve unassisted overall water splitting. Photogenerated electrons are transferred in order through multimediators driven by the electrochemical potential gradient, resulting in efficient charge separation and transportation with enhanced charge transfer rate and reduced charge recombination rate. The integrated system composed of inorganic oxide-based photoanode (BiVO4) and organic polymer-based photocathode (PBDB-T:ITIC:PC71BM) with complementary light absorption, exhibits a solar-to-hydrogen conversion efficiency as high as 4.3%. This work makes a rational design possible by constructing an efficient charge-transfer chain in artificial photosynthesis systems for solar fuel production.
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