As a result of fossil fuel combustion, annual CO2 emissions have increased dramatically since the Industrial Revolution and the atmospheric CO2 level exceeded 410 ppm in 2019. Electrochemical reduction of CO2 may provide a promising solution to the high atmospheric CO2 levels, with CO2 being converted to carbon monoxide, ethylene, or other value-added chemicals. Electrodeposition of Cu, Cu/Ag, and Cu/Sn alloy films by using 3,5-diamino-1,2,4-triazole (DAT) as an electrodeposition inhibitor yield high surface area Cu-based catalysts. All three Cu-based electrodes exhibit high Faradaic efficiency (FE) of CO2 reduction toward C2H4 production. The CuSn-DAT electrode exhibits the highest FE for CO (~90% at -0.4 V) and C2H4 (~60% at -0.8 V) production and high current density (~-225 mA/cm2 at -0.8 V). In situ Surface Enhanced Raman Spectroscopy (SERS) studies in a flow cell obtained from the three Cu-based samples show a correlation between the decreased oxide content on the Cu surface, increased presence of CO, and increased activity for CO and C2H4 production. The CuSn-DAT electrode has the lowest amount of Cu2O and exhibits the highest activity, whereas the Cu-DAT electrode has an increasing Cu2O content and exhibits lower activity as the potential is made negative. These results demonstrate that incorporation of different well-mixed alloy materials provides a way to tune CO2 reduction speciation.

Controlling speciation during CO2 reduction on Cu-alloy electrodes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.