Journal
ACS NANO
Volume 15, Issue 2, Pages 3529-3539Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c00452
Keywords
Bi2WO6; localized surface plasmon resonance; electron doping; CO2 reduction; density functional theory (DFT) calculation
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Funding
- National Natural Science Foundation of China [51872125, 21703083]
- Guangdong Natural Science Funds for Distinguished Young Scholar [2018B030306004]
- GDUPS (2018)
- Regional Joint Foundation in Guangdong Province [2019A1515110210]
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The study successfully constructed plasmonic Bi2WO6 with strong localized surface plasmon resonance (LSPR) through electron doping. Oxygen vacancies on specific sites facilitate photoelectron collection and methane generation in CO2 reduction reaction. The results highlight the importance of V1 sites in enhancing methane production during the CO2-RR process.
Plasmonic Bi2WO6 with strong localized surface plasmon resonance (LSPR) around the 500-1400 region is successfully constructed by electron doping. Oxygen vacancies on W-O-W (V1) and Bi-O-Bi (V2) sites are precisely controlled to obtain Bi2WO6-V1 with LSPR and Bi2WO6-V2 with defect absorption. Density functional theory (DFT) calculation demonstrates that the V1-induced energy state facilitates photoelectron collection for a long lifetime, resulting in LSPR of Bi2WO6. Photoelectron trapping on V1 sites is demonstrated by a single-particle photoluminescence (PL) study, and 93% PL quenching efficiency is observed. With strong LSPR, plasmonic Bi2WO6-V1 exhibits highly selective methane generation with a rate of 9.95 mu mol g(-1) h(-1) during the CO2 reduction reaction (CO2-RR), which is 26-fold higher than 0.37 mu mol g(-1) h(-1) of BiWO3-V2 under UV-visible light irradiation. LSPR-dependent methane generation is confirmed by various photocatalytic results of plasmonic Bi2WO6 with tunable LSPR and different light excitations. Furthermore, the DFT-simulated pathway of CO2-RR and in situ Fourier transform infrared spectra on the surface of Bi2WO6 prove that V1 sites facilitate CH4 generation. Our work provides a strategy to obtain nonmetallic plasmonic materials by electron doping.
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