Abstract

Tuning the facet exposure of Cu could promote the multi-carbon (C2+) products formation in electrocatalytic CO2 reduction. Here we report the design and realization of a dynamic deposition-etch-bombardment method for Cu(100) facets control without using capping agents and polymer binders. The synthesized Cu(100)-rich films lead to a high Faradaic efficiency of 86.5% and a full-cell electricity conversion efficiency of 36.5% towards C2+ products in a flow cell. By further scaling up the electrode into a 25 cm2 membrane electrode assembly system, the overall current can ramp up to 12 A while achieving a single-pass yield of 13.2% for C2+ products. An insight into the influence of Cu facets exposure on intermediates is provided by in situ spectroscopic methods supported by theoretical calculations. The collected information will enable the precise design of CO2 reduction reactions to obtain desired products, a step towards future industrial CO2 refineries.

Highlights

  • Tuning the facet exposure of Cu could promote the multi-carbon (C2+) products formation in electrocatalytic CO2 reduction

  • The colloidally synthesized catalyst needs to be dispersed in a solution containing polymer binders to form a wellmixed ink before being drop-casted on the conductive support to form an electrode, which is not always compatible with the catalytic electrode system due to agglomeration and the peeling-off of catalysts especially when scaling up the electrodes[19,20]

  • We describe the design and realization of a dynamic deposition-etch-bombardment process to produce Cu(100)-rich films as the CO2 reduction electrode in one-step, which could break the limitation of using capping agents while avoiding the issue of catalyst loading faced by conventional methods

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Summary

Introduction

Tuning the facet exposure of Cu could promote the multi-carbon (C2+) products formation in electrocatalytic CO2 reduction. We describe the design and realization of a dynamic deposition-etch-bombardment process to produce Cu(100)-rich films as the CO2 reduction electrode in one-step, which could break the limitation of using capping agents while avoiding the issue of catalyst loading faced by conventional methods. This Cu(100)-rich film yields a full-cell electricity conversion efficiency of 40.5% towards C2+ products in the 4 cm2-. This facile one-step method makes it easier for scaling up electrodes, with a 25 cm[2] electrode exhibiting a 13.2% single-pass yield of C2+

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