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• W3007167403 abstract "Photoconversion of CO2 into fuels completes the carbon neutral cycle in a sustainable society. To exclude the contribution of adventitious carbon, monitoring the time course of 13CO2 conversion into 13C-fuel is essential, but has been rarely reported. In the present work, a composite of Au nanoparticles with ZrO2 was found to be effective in converting 13CO2 into 13CO at a rate of 0.17 μmol h−1 gcat−1 in the presence of H2 and UV–vis light. The detected 12CO as a minor byproduct (11.9 %) was identified as due to adsorbed 12CO2 from the air. The 12C ratio in the total amount of CO2 was evaluated based on a 13CO2 photoexchange reaction (8.7 %). The discrepancy between these values suggested a slower exchange reaction step between the chemisorption site for CO2 reduction and the physisorption site for CO2 compared to the reduction step to CO. Furthermore, based on in-profile kinetic studies using sharp-cut filters and control reactions in the dark, the contribution ratio for CO2 conversion was determined to be via charge separation at the band-gap of ZrO2 (λ < 320 nm): 69 % and via ambient heat (12kT): 31 %. Localized surface plasmon resonance (LSPR) absorption of Au and infrared absorption in the range of λ > 320 nm did not promote catalysis. The LSPR absorption was further investigated by Au L3-edge extended X-ray absorption fine structure analysis. Ambient heat on the Au nanoparticles should have promoted H2 activation enough, supplying protons to the CO2 reduction sites over ZrO2; however, a temperature increase of 26 K on the Au surface was marginal for further H2 activation. CO2 photoconversion with added moisture was also attempted; the CO formation rate using ZrO2 under these conditions was 0.15 μmol h−1 gcat−1. However, 47 % was characterized as 12CO originating from chemisorbed 12CO2, and H2 was also formed at a comparable rate of 0.14 μmol h−1 gcat−1 from a competing reaction. The addition of Au to ZrO2 was found to suppress CO formation and promote H2 formation, and Mg2+ addition to Au–ZrO2 effectively suppressed H2 formation directing to the CO formation." @default.
• W3007167403 created "2020-03-06" @default.
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• W3007167403 date "2020-10-01" @default.
• W3007167403 modified "2023-09-27" @default.
• W3007167403 title "Dual origins of photocatalysis: Light-induced band-gap excitation of zirconium oxide and ambient heat activation of gold to enable 13CO2 photoreduction/conversion" @default.
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• W3007167403 doi "https://doi.org/10.1016/j.cattod.2020.02.040" @default.
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