期刊
ACS CATALYSIS
卷 10, 期 23, 页码 14093-14106出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c03319
关键词
gas-diffusion electrode; triple-phase boundary; double-phase boundary; CO2 reduction; CO2 electrolysis
资金
- U.S. Department of Energy (DOE) [DE-AC36-08GO28308]
- Laboratory Directed Research and Development (LDRD) Program at NREL
- NWO in the form of a Veni Grant
Electrochemical CO2 electrolysis to produce hydrocarbon fuels or material feedstocks offers a renewable alternative to fossilized carbon sources. Gas-diffusion electrodes (GDEs), composed of solid electrocatalysts on porous supports positioned near the interface of a conducting electrolyte and CO2 gas, have been able to demonstrate the substantial current densities needed for future commercialization. These higher reaction rates have often been ascribed to the presence of a three-phase interface, where solid, liquid, and gas provide electrons, water, and CO2, respectively. Conversely, mechanistic work on electrochemical reactions implicates a fully two-phase reaction interface, where gas molecules reach the electrocatalyst's surface by dissolution and diffusion through the electrolyte. Because the discrepancy between an atomistic three-phase versus two-phase reaction has substantial implications for the design of catalysts, gas-diffusion layers, and cell architectures, the nuances of nomenclatures and governing phenomena surrounding the three-phase-region require clarification. Here we outline the macro, micro, and atomistic phenomena occurring within a gas-diffusion electrode to provide a focused discussion on the architecture of the often-discussed three-phase region for CO2 electrolysis. From this information, we comment on the outlook for the broader CO2 electroreduction GDE cell architecture.
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