Microenvironments of Cu catalysts in zero-gap membrane electrode assembly for efficient CO2 electrolysis to C2+ products

Woong Choi, Yongjun Choi, Eunsuh Choi, Hyewon Yun, Wonsang Jung, Woong Hee Lee, Hyung Suk Oh, Da Hye Won, Jonggeol Na, Yun Jeong Hwang

Research output: Contribution to journalArticlepeer-review

Abstract

A zero-gap membrane-electrode assembly (MEA) electrolyzer is a promising design for electrochemical CO2 reduction reactions (eCO2RRs), where gaseous CO2 is directly fed without catholyte. The zero-gap junction between the catalyst and the membrane can have distinct chemical environments and mass transfer properties from the conventional H-type cell but is rarely studied. In this work, we designed an integrated experimental-simulation study in MEA to understand the zero-gap junction and factors to determine the eCO2RR activity to multi-carbon production. We developed a simple synchronous ionomer/catalyst activation step under alkaline conditions to form jagged CuO nanoparticles whose unique morphological evolution facilitates the C2+ chemical production for the zero-gap MEA electrolyzer. Moreover, under gas-fed and high-current density conditions, computational fluid dynamics suggests that the mass transfer limitation of water as a proton source across the catalyst-membrane layer and cathode kinetic overpotential are critical to determining C2+ chemical production in the range of several micrometers. From the chemical-physical understanding, we achieved a high partial current density of 336.5 mA cm−2 and a faradaic efficiency of 67.3% towards C2+ chemicals.

Original languageEnglish
JournalJournal of Materials Chemistry A
DOIs
StateAccepted/In press - 2022

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