Elucidating protonation pathways in CO2 photoreduction using the kinetic isotope effect

Shikang Yin, Yiying Zhou, Zhonghuan Liu, Huijie Wang, Xiaoxue Zhao, Zhi Zhu, Yan Yan () and Pengwei Huo ()
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Shikang Yin: Jiangsu University
Yiying Zhou: Jiangsu University
Zhonghuan Liu: Jiangsu University
Huijie Wang: Jiangsu University
Xiaoxue Zhao: Jiangsu University
Zhi Zhu: Jiangsu University
Yan Yan: Jiangsu University
Pengwei Huo: Jiangsu University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract The surge in anthropogenic CO2 emissions from fossil fuel dependence demands innovative solutions, such as artificial photosynthesis, to convert CO2 into value-added products. Unraveling the CO2 photoreduction mechanism at the molecular level is vital for developing high-performance photocatalysts. Here we show kinetic isotope effect evidence for the contested protonation pathway for CO2 photoreduction on TiO2 nanoparticles, which challenges the long-held assumption of electron-initiated activation. Employing isotopically labeled H2O/D2O and in-situ diffuse reflectance infrared Fourier transform spectroscopy, we observe H+/D+-protonated intermediates on TiO2 nanoparticles and capture their inverse decay kinetic isotope effect. Our findings significantly broaden our understanding of the CO2 uptake mechanism in semiconductor photocatalysts.

Date: 2024
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DOI: 10.1038/s41467-024-44753-x

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