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(Invited) Understanding on the Fundamental Processes of Electrocatalytic Conversion of CO2 to Multi-Carbon Chemicals

作者:Di‐Jia Liu · 发表于:ECS Meeting Abstracts · 年份:2024 · DOI:10.1149/ma2024-02624182mtgabs · 被引用次数:1

The electrochemical CO2 reduction reaction (CO2RR) for chemical production using renewable electricity offers attractive “carbon-neutral” and “carbon-negative” mitigation strategies for greenhouse emission. CO2RR to C2+ chemicals, the compounds containing two or more carbons, represent a particularly interesting topic from both fundamental research as well as practical application points of view. For example, ethanol, ethylene, propanol, etc. are among the most produced chemicals by the industry and are widely used for various applications. Distributive CO2RR by recycling locally emitted CO2 to manufacture these chemicals for the local consumption could substantially reduce the cost of CO2 storage and transport while producing economic income. Electrocatalytic reduction of CO2 involves a fundamental reaction step – proton couple electron transfer (PCET). CO2RR to CO or formic acid requires only two PCET steps, rendering them highly effective with fast kinetics. CO2RR to C2+ chemicals are significantly more challenging due to the rapid escalation of required PCET steps (for example, 12 for ethanol and 18 for propanol), as well as the C-C bond coupling reaction. These increased PCET steps substantially complicate the electrochemical reaction coordinate, leading to a high probability of branching reactions, which lower the single product Faradaic efficiency (FE). [1] At Argonne, we developed an amalgamated lithium metal (ALM) synthesis method of preparing highly selective and ...