Abstract
The electrolysis of dilute CO2 streams suffers from low concentrations of dissolved substrate and its rapid depletion at the electrolyte-electrocatalyst interface. These limitations require first energy-intensive CO2 capture and concentration, before electrolyzers can achieve acceptable performances. For direct electrocatalytic CO2 reduction from low-concentration sources, we in-troduce a strategy that mimics the carboxysome in cyanobacteria by utilizing microcompart-ments with nanoconfined and concentrated enzymes in a porous electrode. A carbonic anhy-drase accelerates CO2 hydration kinetics and minimizes substrate depletion by making all dis-solved carbon available for utilization, while a highly efficient formate dehydrogenase reduces CO2 cleanly to formate; down to even atmospheric concentrations of CO2. This bio-inspired concept demonstrates that the carboxysome provides a viable blueprint and strategy to achieve the reduction of low-concentration CO2 streams to chemicals.
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