Covalent Immobilization of a Molecular Catalyst on Cu2O Photocathodes for CO2 Reduction
- 4 February 2016
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 138 (6), 1938-1946
- https://doi.org/10.1021/jacs.5b12157
Abstract
Sunlight-driven CO2 reduction is a promising way to close the anthropogenic carbon cycle. Integrating light harvester and electrocatalyst functions into a single photoelectrode, which converts solar energy and CO2 directly into reduced carbon species, is under extensive investigation. The immobilization of rhenium-containing CO2 reduction catalysts on the surface of a protected Cu2O-based photocathode allows for the design of a photofunctional unit combining the advantages of molecular catalysts with inorganic photoabsorbers. To achieve large current densities, a nanostructured TiO2 scaffold, processed at low temperature, was deposited on the surface of protected Cu2O photocathodes. This led to a 40-fold enhancement of the catalytic photocurrent as compared to planar devices, resulting in the sunlight-driven evolution of CO at large current densities and with high selectivity. Potentiodynamic and spectroelectrochemical measurements point toward a similar mechanism for the catalyst in the bound and unbound form, whereas no significant production of CO was observed from the scaffold in the absence of a molecular catalyst.Keywords
Funding Information
- Siemens
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