Abstract
To help achieve carbon neutrality by 2050, electrochemical CO2 reduction (eCO2R) is attractive as it can both reduce fossil fuel dependency and afford valuable industrial chemicals using renewable energy. While the low solubility of CO2 limits eCO2R viability in batch cells, flow cells using a gas-diffusion electrode (GDE) boost mass transport of CO2 to the electrocatalyst, attaining viable performance toward simple products like CO. However, eCO2R to the more valuable triple-carbon (C3) oxygenates (acetone, n-propanol and isopropanol), which are otherwise produced with high emissions, remains challenging. Most state-of-the-art electrocatalysts toward C3 oxygenates have so far been developed in batch cells, attaining overall poor performance in flow cells. The objective of this project is to design an improved eCO2R electrocatalyst for C3 oxygenates in a flow cell. By using electron tomography and other HR-(S)TEM techniques to reveal the 3D structure of highly modular porous carbon electrocatalysts, structural correlations with electrochemical performance will be used to rationally optimise these nanomaterials to flow cell conditions. With further optimisation supported by in-situ characterisation, the final electrocatalyst will achieve breakthrough selectivity of ? 25% to C3 oxygenates at industrial current densities ? 200 mA/cm^2. As such, this project will provide a key step forward to future industrially viable C3 oxygenate production via eCO2R.
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