Enhanced Carbon Monoxide Electroreduction to &gt;1 A cm <sup>−2</sup> C <sub>2+</sub> Products Using Copper Catalysts Dispersed on MgAl Layered Double Hydroxide Nanosheet House‐of‐Cards Scaffolds

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Abstract

Cu catalysts are most apt for reducing CO ₍₂₎ to multi‐carbon products in aqueous electrolytes. To enhance the product yield, we can increase the overpotential and the catalyst mass loading. However, these approaches can cause inadequate mass transport of CO ₍₂₎ to the catalytic sites, which will then lead to H ₂ evolution dominating the product selectivity. Herein, we use a MgAl LDH nanosheet ‘house‐of‐cards’ scaffold to disperse CuO‐derived Cu (OD‐Cu). With this support‐catalyst design, at −0.7 V _RHE, CO could be reduced to C ₂₊ products with a current density ( j _C2+) of −1251 mA cm ⁻². This is 14× that of the j _C2+ shown by unsupported OD‐Cu. The current densities of C ₂₊ alcohols and C ₂H ₄ were also high at −369 and −816 mA cm ⁻² respectively. We propose that the porosity of the LDH nanosheet scaffold enhances CO diffusion through the Cu sites. The CO reduction rate can thus be increased, while minimizing H ₂ evolution, even when high catalyst loadings and large overpotentials are used.

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Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte

Stephanie A Nitopi, Erlend Bertheussen, Soren B Scott … (2019)

To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene and ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors that impact CO2R activity and selectivity, including the catalyst surface structure, morphology, composition, the choice of electrolyte ions and pH, and the electrochemical cell design. Many of these factors are often intertwined, which can complicate catalyst discovery and design efforts. Here we take a broad and historical view of these different aspects and their complex interplay in CO2R catalysis on Cu, with the purpose of providing new insights, critical evaluations, and guidance to the field with regard to research directions and best practices. First, we describe the various experimental probes and complementary theoretical methods that have been used to discern the mechanisms by which products are formed, and next we present our current understanding of the complex reaction networks for CO2R on Cu. We then analyze two key methods that have been used in attempts to alter the activity and selectivity of Cu: nanostructuring and the formation of bimetallic electrodes. Finally, we offer some perspectives on the future outlook for electrochemical CO2R.