期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 40, 页码 13522-13527出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201300764
关键词
CO2 reduction; iron; photoelectrocatalysis; porphyrins; p-type silicon
资金
- EPSRC [F047878/1]
- EPSRC (SolarCap consortium)
- University of Hail, Saudi Arabia
- Engineering and Physical Sciences Research Council [EP/F047878/1] Funding Source: researchfish
- EPSRC [EP/F047878/1] Funding Source: UKRI
Photoelectrocatalytic conversion of CO2 to CO can be driven at a boron-doped, hydrogen terminated, p-type silicon electrode using a meso-tetraphenylporphyrin Fe-III chloride in the presence of CF3CH2OH as a proton source and 0.1M [NBu4][BF4]/MeCN/5% DMF (v/v) as the electrolyte. Under illumination with polychromatic light, the photoelectrocatalysis operates with a photovoltage of about 650mV positive of that for the dark reaction. Carbon monoxide is produced with a current efficiency >90% and with a high selectivity over H-2 formation. Photoelectrochemical current densities of 3mAcm(-2) at -1.1V versus SCE are typical, and 175 turnovers have been attained over a 6h period. Cyclic voltammetric data are consistent with a turnover frequency of =1.03x10(4)s(-1) for the electrocatalysis in the dark on vitreous carbon at a potential of -1.85V versus SCE.
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