4.8 Article

Metallic AgInS2 nanocrystals with sulfur vacancies boost atmospheric CO2 photoreduction under near-infrared light illumination

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DOI: 10.1016/j.apcatb.2023.122763

Keywords

Vacancy; AgInS2; Metallic catalyst; CO2 photoreduction; Near-infrared light

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This study investigates the influence of vacancy engineering on intrinsic CO2 photoreduction with low photon energy directly from air. The authors designed a metallic photocatalyst, V-S-AgInS2 nanocrystals, which exhibited superior atmospheric CO2 reduction performance under near-infrared light. The presence of sulfur vacancies and metallic characteristics in the nanocrystals resulted in extended spectrum absorption and efficient charge carrier separation. The experimental and theoretical results showed that charge delocalization around the vacancy-induced dual sites promoted CO production while inhibiting the formation of CHO intermediates. Consequently, the metallic VS-AgInS2 nanocrystals achieved nearly 100% selective CO production under NIR irradiation.
Unraveling the function of vacancy engineering in influencing the intrinsic CO2 photoreduction with low photon energy directly from air remains a significant challenge. Here, a metallic photocatalyst, ultrafine AgInS2 nanocrystals with sulfur vacancies (V-S-AgInS2) is designed to exhibit superior atmospheric CO2 reduction performance under near-infrared (NIR) light. Theoretical calculations reveal that the presence of sulfur vacancies and metallic characteristics result in extended spectrum absorption to the NIR region and efficient separation of charge carriers. As evidenced by In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) experiment and theoretical calculations, the unique properties of charge delocalization around the vacancy-induced dual sites at AgInS2 nanocrystals contribute to COOH* intermediates for CO production while simultaneously inhibiting the formation of CHO* intermediates. Consequently, the metallic VS-AgInS2 nanocrystals demonstrate nearly 100% selective CO production with a rate of 8.04 mu mol g(-1) h(-1) under NIR irradiation, even directly from atmospheric CO2 in the air.

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