期刊
NATURE CATALYSIS
卷 2, 期 4, 页码 354-365出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-019-0254-2
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资金
- Woolf Fisher Trust in New Zealand
- Christian Doppler Research Association (Austrian Federal Ministry for Digital and Economic Affairs)
- Christian Doppler Research Association (National Foundation for Research, Technology and Development)
- OMV Group
- ERC Consolidator Grant 'MatEnSAP' [682833]
- European Union's Horizon2020 research and innovation programme (Marie Sklodowska-Curie fellowship) [GAN 701192]
- National Research Foundation via the Creative Research Initiative Center (Republic of Korea) [NRF-2015R1A3A2066191]
The selective reduction of CO2 with inexpensive solar-driven photoelectrochemical devices is a contemporary challenge in the quest for renewable fuel production. Here, we report a molecular catalyst-based photocathode assembled from precious-metal-free components that is active towards aqueous CO2 reduction. The reported photocathode is based on a phosphonated cobalt bis(terpyridine) catalyst that is interfaced via a mesoporous TiO2 scaffold with a light-harvesting p-type silicon electrode. The hybrid photoelectrode reduces CO2 to CO in both organic-water and purely aqueous conditions, achieving a turnover number of similar to 330 and maintaining stable activity for more than one day. Critically, in-depth electrochemical as well as in situ resonance Raman and infrared spectroelectrochemical investigations alluded to a catalytic mechanism that differs to that reported for the soluble metal bis(terpyridine) catalyst as the consequence of the immobilization. In addition, it further unlocks an earlier catalytic onset and better electrocatalytic performance while enabling aqueous CO2 reduction with the reported photocathode.
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