While metallic copper has been recognized for its potential in eCO2RR, traditional polycrystalline Cu electrodes often struggle with poor selectivity due to a variety of reaction intermediates and complex pathways. The development of a cost-effective and efficient Cu catalyst with improved selectivity has remained a significant challenge.
To overcome these obstacles, Prof. Shen's team developed a modified Cu electrode by coating it with poly(a-ethyl cyanoacrylate) (PECA). This polymer, featuring electron-accepting cyano (-C=N) and ester (-COOR) groups, was created through the anionic polymerization of surface-adhered ECA. The modification stabilizes key intermediates, leading to a more selective production of C2+ products during the eCO2RR process.
Compared to traditional Cu electrodes, the PECA-coated Cu electrode demonstrated significantly better performance. It achieved a Faradaic efficiency (FE) of 72.6% at -1.1 V vs. RHE and, in a flow cell setup, maintained a high FE of 76.3% with a current density of -145.4 mA cm-2 at -0.9 V vs. RHE.
Through a combination of electrochemical analysis, in-situ spectral investigations, and theoretical calculations, the researchers found that the PECA coating alters the interfacial electron distribution and raises the energy level of the d-band in Cu active sites. This modification reduces H adsorption and stabilizes CO adsorption, promoting the necessary C-C coupling for the selective formation of C2+ products.
This study provides a valuable strategy for designing surface-modified electrocatalysts that can steer the adsorption behaviors of reaction intermediates, enhancing both the activity and selectivity of eCO2RR towards multicarbon products.
Research Report:Polyacrylate modified Cu electrode for selective electrochemical CO2 reduction towards multicarbon products
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