Role of water and carbonates in photocatalytic transformation of CO{sub 2} to CH{sub 4} on titania.
- Center for Nanoscale Materials
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 {center_dot}OH radicals (oxidation product) from water, and CO{sub 3}{sup -} radical anions (oxidation product) from carbonates, was detected in CO{sub 2}-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, {center_dot}OCH{sub 3}, and methyl, {center_dot}CH{sub 3}, radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO{sub 2} on the surface of TiO{sub 2} is supported by the results of first-principles calculations.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- DOE Contract Number:
- DE-AC02-06CH11357
- OSTI ID:
- 1012807
- Report Number(s):
- ANL/CSE/JA-69200; TRN: US201110%%365
- Journal Information:
- J. Am. Chem. Soc., Vol. 133, Issue Feb, 24, 2011
- Country of Publication:
- United States
- Language:
- ENGLISH
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