Role of Water and Carbonates in Photocatalytic Transformation of CO2 to CH4 on Titania
Journal of the American Chemical Society2011Vol. 133(11), pp. 3964–3971
Citations Over TimeTop 1% of 2011 papers
Nada M. Dimitrijević, Baiju Kizhakkekilikoodayil Vijayan, Oleg G. Poluektov, Tijana Rajh, Kimberly A. Gray, Haiying He, Peter Zapol
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 CO(3)(-) radical anions (oxidation product) from carbonates, was detected in CO(2)-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, (•)OCH(3), and methyl, (•)CH(3), radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO(2) on the surface of TiO(2) is supported by the results of first-principles calculations.
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