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Selective photocatalytic CO$_2$ reduction in water through anchoring of a molecular Ni catalyst on CdS nanocrystals

Accepted version
Peer-reviewed

Type

Article

Change log

Authors

Orchard, K 
Dalle, K 

Abstract

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 H2 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 cm2, λ > 400 nm, pH 6.7, 25 °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 H2 evolution in aqueous solution.

Description

Keywords

3403 Macromolecular and Materials Chemistry, 34 Chemical Sciences, 3406 Physical Chemistry, 40 Engineering, 4004 Chemical Engineering, 4018 Nanotechnology, 7 Affordable and Clean Energy, 13 Climate Action

Journal Title

Journal of the American Chemical Society

Conference Name

Journal ISSN

0002-7863
1520-5126

Volume Title

139

Publisher

American Chemical Society
Sponsorship
Isaac Newton Trust (1238(k))
Christian Doppler Forschungsgesellschaft (unknown)
Tohoku University (unknown)
Christian Doppler Research Association, OMV group, Isaac Newton Trust, the German Research Foundation, the World Premier International Research Center Initiative, MEXT, Japan