Role of water and carbonates in photocatalytic transformation of CO 2 to CH4 on titania

Nada M. Dimitrijevic; Baiju K. Vijayan; Oleg G. Poluektov; Tijana Rajh; Kimberly A. Gray; Haiying He; Peter Zapol

doi:10.1021/ja108791u

Role of water and carbonates in photocatalytic transformation of CO ₂ to CH₄ on titania

Nada M. Dimitrijevic, Baiju K. Vijayan, Oleg G. Poluektov, Tijana Rajh, Kimberly A. Gray, Haiying He, Peter Zapol

Civil and Environmental Engineering

Research output: Contribution to journal › Article › peer-review

434 Scopus citations

Abstract

Using the electron paramagnetic resonance technique, we have elucidated the multiple roles of water and carbonates in the overall photocatalytic reduction of carbon dioxide to methane over titania nanoparticles. The formation of H atoms (reduction product) and •OH radicals (oxidation product) from water, and CO₃^- radical anions (oxidation product) from carbonates, was detected in CO₂-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, •OCH₃, and methyl, •CH₃, radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO₂ on the surface of TiO₂ is supported by the results of first-principles calculations.

Original language	English (US)
Pages (from-to)	3964-3971
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	133
Issue number	11
DOIs	https://doi.org/10.1021/ja108791u
State	Published - Mar 23 2011

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/ja108791u

Cite this

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abstract = "Using the electron paramagnetic resonance technique, we have elucidated the multiple roles of water and carbonates in the overall photocatalytic reduction of carbon dioxide to methane over titania nanoparticles. The formation of H atoms (reduction product) and •OH radicals (oxidation product) from water, and CO3- radical anions (oxidation product) from carbonates, was detected in CO2-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, •OCH3, and methyl, •CH3, radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO2 on the surface of TiO2 is supported by the results of first-principles calculations.",

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AU - Dimitrijevic, Nada M.

AU - Vijayan, Baiju K.

AU - Poluektov, Oleg G.

AU - Rajh, Tijana

AU - Gray, Kimberly A.

AU - He, Haiying

AU - Zapol, Peter

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