Journal
ACS MATERIALS LETTERS
Volume 3, Issue 4, Pages 364-371Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsmaterialslett.1c00091
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Funding
- National Nature Science Foundation of China [21671113, 51872147]
- Natural Science Foundation of Henan Province [202300410298]
- 111 Project [D20015]
- Program for Innovative Research Team of Science and Technology in the University of Henan Province [19IRTSTHN025]
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Single-atom active sites engineering can enhance charge separation and CO2 activation for high-performance CO2 reduction. The proposed Bi4O5I2 catalyst with single-atom Fe implantation shows exceptional CO and CH4 production rates, outperforming other photocatalysts reported to date.
Insufficient separation of photogenerated electron-hole and feeble CO2 activation remain the main obstacles in the access to high-performance CO2 reduction nowadays. Single-atom active sites engineering could be an efficient method through simultaneously promoting charge separation and CO2 activation. Herein, a model of Bi4O5I2 with single-atom Fe implanting and accompanying Bi decorating on surface is proposed to boost the performance. The single-atom Fe implantation decreases the value of surface work function, allowing the fast transition of photon-generated electrons from the surface of catalyst to CO2 molecule. In situ Fourier transform infrared (FT-IR) spectra, CO2 adsorption measurements, density functional theory (DFT) calculations, and efficient CO2 activation are realized on as-established single-atom catalyst. An exceptional yield of CO (23.77 mu mol g(-1) h(-1)) and CH4 production (4.98 mu mol g(-1) h(-1)) is acquired over optimized Bi4O5I2-Fe30 with 1.09 wt % of single-atom Fe, superior to Bi4O5I2, and most other reported photocatalysts. The work paves a insight into rational design of photocatalysts toward simultaneously facilitating carrier separation and CO2 activation from the angle of atom single metal.
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