Copper hydroxide/basic copper salt derived Cu0 with a clear grain boundary for selective electrocatalytic CO2 reduction to produce multicarbon products
Journal of materials chemistry. A, Materials for energy and sustainability(2023)
摘要
Electrocatalytic CO2 reduction (ECR) is one of the most promising ways to mitigate CO2 and fuel production, and multicarbon products (C2+) with high chemical value attract lots of interest. Cu is a unique electrocatalyst that can convert CO2 to multicarbon products, but with limited selectivity and activity. Here, aiming for a clear Cu-0 nanoparticle structure with a clear grain boundary, we report a simple and effective method of Cu(OH)(2)/basic copper sulphate compound material synthesis, which is in situ reduced to Cu-0 nanoparticles with a clear grain boundary (GB) during the ECR process. The Cu(OH)(2)/basic copper sulphate-derived Cu nanoparticles show a high C2+ faradaic efficiency (FE) of 81% at -1.2 V vs. RHE, which surpasses that of state-of-the-art Cu-based catalysts evaluated in an H-type cell. Extending the method to other basic copper salts (BCS), we successfully synthesized three other Cu(OH)(2)/BCS species (nitrate, carbonate and chloride), which were also converted to Cu-0 with a clear grain boundary during ECR. DFT calculation results reveal that the GB sites could effectively decrease the energy barrier of the reactant CO2 adsorption and critical C-C coupling steps, which endows the derived Cu electrocatalyst with high selectivity for C2H4 and C2+ products.
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