<p>Carbon capture, recovery and conversion are typically done by three separate steps, which notably increases the total energy consumption and capital costs. Here we propose to indirectly convert (bi)carbonates, which are carbon-rich sorbents in alkaline carbon capture, into valuable chemicals in a porous solid electrolyte (PSE) electrochemical CO<sub>2</sub> reduction (CO<sub>2</sub>RR) reactor while eliminating the energy-intensive CO<sub>2</sub> recovery step. Specifically, direct feeding of (bi)carbonates into the PSE layer while performing CO<sub>2</sub>RR allows simultaneous CO<sub>2</sub> regeneration within the PSE chamber. Impressive electrochemical performance was demonstrated, with up to 96% formate Faradaic efficiency, 95% CO<sub>2</sub> recovery efficiency and 86% bicarbonate-to-formate conversion. Reactor versatility allowed us to obtain up to 5.0 M formate, ~50% higher than bicarbonate solubility and C<sub>2+</sub> products with 73% selectivity, setting the state of the art for bicarbonate-fed CO<sub>2</sub>RR. Operating for at least 100 hours at 100 mA cm<sup>−</sup><sup>2</sup> averaging 82% CO<sub>2</sub> recovery and 89% Faradaic efficiencies, our reactor adds economic value to alkaline carbon capture and CO<sub>2</sub> conversion, bringing both closer to practical implementation.</p>

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Energy-efficient indirect (bi)carbonate electroreduction in a porous solid electrolyte reactor

  • Valery Okatenko,
  • Ahmad Elgazzar,
  • Anna Loiudice,
  • Raffaella Buonsanti,
  • Haotian Wang

摘要

Carbon capture, recovery and conversion are typically done by three separate steps, which notably increases the total energy consumption and capital costs. Here we propose to indirectly convert (bi)carbonates, which are carbon-rich sorbents in alkaline carbon capture, into valuable chemicals in a porous solid electrolyte (PSE) electrochemical CO2 reduction (CO2RR) reactor while eliminating the energy-intensive CO2 recovery step. Specifically, direct feeding of (bi)carbonates into the PSE layer while performing CO2RR allows simultaneous CO2 regeneration within the PSE chamber. Impressive electrochemical performance was demonstrated, with up to 96% formate Faradaic efficiency, 95% CO2 recovery efficiency and 86% bicarbonate-to-formate conversion. Reactor versatility allowed us to obtain up to 5.0 M formate, ~50% higher than bicarbonate solubility and C2+ products with 73% selectivity, setting the state of the art for bicarbonate-fed CO2RR. Operating for at least 100 hours at 100 mA cm2 averaging 82% CO2 recovery and 89% Faradaic efficiencies, our reactor adds economic value to alkaline carbon capture and CO2 conversion, bringing both closer to practical implementation.