Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-16847-9
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Funding
- National Key Projects for Fundamental Research and Development of China [2017YFA0206904, 2017YFA0206900, 2016YFB0600901, 2018YFB1502002]
- National Natural Science Foundation of China [51825205, U1662118, 51772305, 51572270, 21871279, 21802154, 21902168]
- Beijing Natural Science Foundation [2191002, 2194089, 2182078]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Beijing Municipal Science and Technology Project [Z181100005118007]
- Royal Society-Newton Advanced Fellowship [NA170422]
- International Partnership Program of Chinese Academy of Sciences [GJHZ1819, GJHZ201974]
- K. C. Wong Education Foundation
- Youth Innovation Promotion Association of the CAS
- University of Auckland Faculty Research Development Fund
- Energy Education Trust of New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology
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The electrochemical CO2 reduction reaction (CO2RR) represents a very promising future strategy for synthesizing carbon-containing chemicals in a more sustainable way. In spite of great progress in electrocatalyst design over the last decade, the critical role of wettability-controlled interfacial structures for CO2RR remains largely unexplored. Here, we systematically modify the structure of gas-liquid-solid interfaces over a typical Au/C gas diffusion electrode through wettability modification to reveal its contribution to interfacial CO2 transportation and electroreduction. Based on confocal laser scanning microscopy measurements, the Cassie-Wenzel coexistence state is demonstrated to be the ideal three phase structure for continuous CO2 supply from gas phase to Au active sites at high current densities. The pivotal role of interfacial structure for the stabilization of the interfacial CO2 concentration during CO2RR is quantitatively analysed through a newly-developed in-situ fluorescence electrochemical spectroscopic method, pinpointing the necessary CO2 mass transfer conditions for CO2RR operation at high current densities.
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