Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 317, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121727
Keywords
Van der Waals heterojunction; Black phosphorus; Bi 19 Br 3 S 27 composite; Activated hydrogen; CO 2 photoreduction; Photocatalysis
Funding
- Outstanding Talent Research Fund of Zhengzhou University
- China Postdoctoral Science Foundation [2020TQ0277, 2020M682328]
- Central Plains Science and Technology Innovation Leader Project [214200510006]
- Postdoctoral Science Foundation of Henan Province [202002010]
- National Supercomputing Center in Zhengzhou
- Hefei Advanced Computing Center
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In this study, the supply of activated hydrogen (H*) in photocatalytic CO2 reduction is improved by fabricating a heterojunction of black phosphorus (BP) nanosheets and Bi19Br3S27 nanorods (BP/BBS). This heterojunction enhances the separation of photogenerated carriers and decreases the rate-limiting H* formation step, ensuring efficient CO2 reduction. The optimized BP/BBS heterojunction achieves an enhanced generation rate of solar fuels in both liquid and gas-solid phase systems.
Photocatalytic CO2 reduction (PCC) into solar fuels has been identified as a green avenue for carbon emission reduction. The reactions are usually restricted by the competitive hydrogen production reactions so that the acquisition and utilization of activated hydrogen (H*) in photocatalytic CO(2 )reduction are hard to guarantee. Herein, heterojunction engineering, regarding amendatory H* supply and balancing hydrogen production re-actions simultaneously, for enhancing PCC is achieved by fabricating black phosphorus (BP) nanosheets sup-ported on Bi19Br3S27 nanorods (BP/BBS). Density functional theory calculations united with experimental researches confirm the charge transfer conforms to S-scheme mechanism, which guarantee the efficient sepa-ration of photogenerated carriers to facilitate CO2 photoreduction. Free energy analysis reveals the formation of BP/BBS heterojunction changes the active sites from BBS to BP, which decrease the rate-limiting H* formation step from 1.94 (on BBS) to 1.13 eV (BP/BBS heterojunction), ensuring the supply of activated H* for PCC. We found that the heat of the PCC is conducive to dominant protonation of CO2 not H* desorption, which can greatly improve the reduction efficiency of CO2. As a result, the optimized BP/BBS heterojunction achieves an enhanced generation rate of solar fuels in liquid or gas-solid phase system with CO generation rate of 395.7 and 35.4 mu mol g(-1) catalyst, respectively. This work provides an efficient strategy to achieve the supply of activated H* for PCC and other photochemical process.
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