<p>Electrochemical CO<sub>2</sub> reduction (ECR) in acidic electrolytes minimizes CO<sub>2</sub> loss and carbonate formation issues, allowing for high CO<sub>2</sub> utilization efficiency and showing good potential for practical CO<sub>2</sub> upgrading applications. However, in the membrane-based electrolyzer, the proton transfer efficiency across the membrane from the anolyte to the catholyte is crucial for the stability of the catholyte pH in acidic ECR, especially at high current density and during long-term electrolysis. Here, we investigate the effects of proton transfer efficiency and salt precipitation in different acidic ECR electrolyzer and propose a membrane-free CO<sub>2</sub> hydrogenation electrolyzer, which couple CO<sub>2</sub> reduction and hydrogen oxidation. This electrolyzer design effectively maintains a stable electrolyte pH during long-term electrolysis, and simultaneously achieves high Faradaic efficiency for HCOOH production, high single-pass carbon utilization efficiency, and a lower cell voltage. At a current density of 100 mA cm<sup>−2</sup>, the system requires only 1.7 V to achieve a 90% HCOOH Faradaic efficiency and demonstrates stable operation for 208 hours.</p>

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Membrane-free CO2 hydrogenation electrolyzer for salt precipitation management in acidic electrochemical CO2 reduction

  • Yumin Da,
  • Lei Fan,
  • Wenlong Wang,
  • Rui Jiang,
  • Haotian Lu,
  • Hongqiang Jin,
  • Ganwen Chen,
  • Chonglai Jiang,
  • Chenrui Ji,
  • Xiang Chen,
  • Tong Zhu,
  • Zhe Wu,
  • Wei Chen

摘要

Electrochemical CO2 reduction (ECR) in acidic electrolytes minimizes CO2 loss and carbonate formation issues, allowing for high CO2 utilization efficiency and showing good potential for practical CO2 upgrading applications. However, in the membrane-based electrolyzer, the proton transfer efficiency across the membrane from the anolyte to the catholyte is crucial for the stability of the catholyte pH in acidic ECR, especially at high current density and during long-term electrolysis. Here, we investigate the effects of proton transfer efficiency and salt precipitation in different acidic ECR electrolyzer and propose a membrane-free CO2 hydrogenation electrolyzer, which couple CO2 reduction and hydrogen oxidation. This electrolyzer design effectively maintains a stable electrolyte pH during long-term electrolysis, and simultaneously achieves high Faradaic efficiency for HCOOH production, high single-pass carbon utilization efficiency, and a lower cell voltage. At a current density of 100 mA cm−2, the system requires only 1.7 V to achieve a 90% HCOOH Faradaic efficiency and demonstrates stable operation for 208 hours.