Efficient wettability-controlled electroreduction of CO2 to CO at Au/C interfaces

Abstract

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.

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

“…As a representative greenhouse gas, carbon dioxide (CO 2 ) has brought out serious environmental problems needing to solve urgently 1 , 2 . Photocatalytic CO 2 conversion technology has attracted extensive interest, since the conversion of CO 2 into high value-added chemicals could potentially be achieved under relatively mild conditions, which facilitates its resource utilization 3 , 4 .…”

The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO2 Electroreduction

“…[8][9][10] The utilization of noble-metal catalysts for electroreduction of CO 2 to CO has made excellent progress, such as Au, Ag. [11][12][13] It is well known that the scarcity and cost of precious metals limit their industrial applications. To date, Cu-based catalysts have most abundant product (e. g., HCOOH, CH 3 CH 2 OH, C 2 H 6 , C 2 H 4 ) in the prior reports.…”

“…In recent years, a large number of efforts have been used in the studies of electrocatalysts with excellent properties [8–10] . The utilization of noble‐metal catalysts for electroreduction of CO 2 to CO has made excellent progress, such as Au, Ag [11–13] . It is well known that the scarcity and cost of precious metals limit their industrial applications.…”

Flooded by Success: On the Role of Electrode Wettability in CO2 Electrolyzers That Generate Liquid Products

“…40,41 Despite the obscurations introduced by roughness and entrapped fluids when determining quantitative measures of wettability on porous substrates, droplet based-protocols are widely practiced to evaluate the resistance of textiles and other electrochemically functional materials to wetting. [42][43][44][45][46][47]…”