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<p>The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) relies heavily on the surrounding microenvironment to promote formation of desirable multicarbon (C<sub>2+</sub>) products. However, microenvironment control to achieve high C<sub>2+</sub> yields at industrially relevant current densities remains a crucial challenge. We report that chitosan, cellulose and chitin biopolymer coatings on CO<sub>2</sub>RR electrocatalysts enhance the microenvironment by increasing local CO<sub>2</sub>/CO concentration, reducing local water activity and providing suitable ion conductivity and local pH. This facile approach achieves C<sub>2+</sub> Faradaic efficiencies of 90 ± 1.7% at 1.6 A cm<sup>−2</sup> and C<sub>2+</sub> Faradaic efficiency = 83 ± 3.2% at 2.2 A cm<sup>−2</sup> with a formation rate of 5,926 μmol h<sup>−1</sup> cm<sup>−2</sup>. Importantly, within the cathode, these ion-conductive hydrophilic biopolymers can fully substitute traditional hydrophobic ionomers/binders, such as Nafion, challenging previous assumptions about the non-viability of hydrophilic materials for selective CO<sub>2</sub>RR due to excess interfacial H<sub>2</sub>O. These findings unveil key insights into microenvironment design to enhance C–C coupling through a simple method.</p>

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A scalable, biopolymer-based microenvironment for electrochemical CO2 conversion to multicarbon products with current densities over 2 A cm−2

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月17日

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  • Chaolong Wei,
  • Suhwan Yoo,
  • Yan Li,
  • Haibin Ma,
  • Yaqi Cheng,
  • Yao Wu,
  • Guangxin Sun,
  • Caiwei Zhang,
  • Qian He,
  • Tiras Y. Lin,
  • Boon Siang Yeo,
  • Joel B. Varley,
  • Yun Jeong Hwang,
  • Chunnian He,
  • Andrew Barnabas Wong

摘要

The electrochemical CO2 reduction reaction (CO2RR) relies heavily on the surrounding microenvironment to promote formation of desirable multicarbon (C2+) products. However, microenvironment control to achieve high C2+ yields at industrially relevant current densities remains a crucial challenge. We report that chitosan, cellulose and chitin biopolymer coatings on CO2RR electrocatalysts enhance the microenvironment by increasing local CO2/CO concentration, reducing local water activity and providing suitable ion conductivity and local pH. This facile approach achieves C2+ Faradaic efficiencies of 90 ± 1.7% at 1.6 A cm−2 and C2+ Faradaic efficiency = 83 ± 3.2% at 2.2 A cm−2 with a formation rate of 5,926 μmol h−1 cm−2. Importantly, within the cathode, these ion-conductive hydrophilic biopolymers can fully substitute traditional hydrophobic ionomers/binders, such as Nafion, challenging previous assumptions about the non-viability of hydrophilic materials for selective CO2RR due to excess interfacial H2O. These findings unveil key insights into microenvironment design to enhance C–C coupling through a simple method.