Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 21, Pages 7217-7223Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b00369
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Funding
- Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy)
- Christian Doppler Research Association (National Foundation for Research, Technology and Development)
- OMV Group
- Isaac Newton Trust [12.38/k]
- German Research Foundation [KU 3077/2-1]
- World Premier International Research Center Initiative (WPI), MEXT, Japan
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Photocatalytic conversion of CO2 into carbonaceous feedstock chemicals is a promising strategy to mitigate greenhouse gas emissions and simultaneously store solar energy in chemical form. Photocatalysts for this transformation are typically based on precious metals and operate in nonaqueous solvents to suppress competing H-2 generation. In this work, we demonstrate selective visible-light-driven CO2 reduction in water using a synthetic photocatalyst system that is entirely free of precious metals. We present a series of self-assembled nickel terpyridine complexes as electrocatalysts for the reduction of CO2 to CO in organic media. Immobilization on CdS quantum dots allows these catalysts to be active in purely aqueous solution and photocatalytically reduce CO2 with >90% selectivity under UV-filtered simulated solar light irradiation (AM 1.5G, 100 mW cm(-2), lambda > 400 nm, pH 6.7, 25 degrees C). Correlation between catalyst immobilization efficiency and product selectivity shows that anchoring the molecular catalyst on the semiconductor surface is key in controlling the selectivity for CO2 reduction over H-2 evolution in aqueous solution
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