Enhanced CO₂ Electroreduction to Ethylene on Laser-Synthesized Copper Phyllosilicate Catalysts

High Resolution Image Download MS PowerPoint Slide Carbon dioxide electrochemical reduction (CO 2 ECR) to ethylene is a promising means of simultaneously mitigating CO 2 emissions and producing an important feedstock for industrial, environmental, and agricultural sectors without petroleum. However, developing CO 2 ECR catalysts with high ethylene selectivity remains a challenge. This work reports the synthesis of copper phyllosilicate (CuPS) CO 2 ECR catalysts using the nonequilibrium reactive laser ablation in liquid (RLAL) technique. Compared to CuPS synthesized through conventional ammonia evaporation (CuPS-AE), which only contained Cu 2+ species, the RLAL-synthesized CuPS catalysts had higher Cu loading and contained reduced copper (Cu + ). Cu-PS synthesized using 30 fs laser pulses (CuPS-fs) contained nearly 50% more Cu + than CuPS synthesized using 4 ps pulses (CuPS-ps), along with a higher concentration of crystalline Cu 2 O phases within the amorphous CuPS network. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements showed a higher fraction of CO 2 adsorption on copper sites as compared to oxygen functional group sites for the CuPS-fs catalyst. CO 2 ECR measurements showed exceptional ethylene selectivity for the CuPS-fs catalyst, reaching 84% Faradaic efficiency (FE) at −1.1 V vs RHE, compared to 29 and 16% for the CuPS-ps and CuPS-AE catalysts, respectively. Moreover, the CuPS-fs catalyst exhibited exceptional stability, maintaining more than 80% FE to ethylene and 10 mA cm –2 current density over 30 h on stream.