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

Wei, Chaolong [Tianjin Univ. (China); National University of Singapore (Singapore)] (ORCID:0009000761505060); Yoo, Suhwan [Seoul National Univ. (Korea, Republic of)]; Li, Yan [National University of Singapore (Singapore)]; Ma, Haibin [National University of Singapore (Singapore)]; Cheng, Yaqi [National University of Singapore (Singapore)] (ORCID:0000000307125984); Wu, Yao [National University of Singapore (Singapore)] (ORCID:0009000514237097); Sun, Guangxin [Tianjin Univ. (China); National University of Singapore (Singapore)]; Zhang, Caiwei [National University of Singapore (Singapore)]; He, Qian [National University of Singapore (Singapore)] (ORCID:0000000348913581); Lin, Tiras Y. [Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Computational Engineering Division] (ORCID:0000000233779933); Yeo, Boon Siang [National University of Singapore (Singapore)] (ORCID:0000000316090867); Varley, Joel B. [Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Materials Science Division; Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF)]; Hwang, Yun Jeong [Seoul National Univ. (Korea, Republic of)] (ORCID:0000000209801758); He, Chunnian [Tianjin Univ. (China)] (ORCID:0000000257686598); Wong, Andrew Barnabas [National University of Singapore (Singapore)] (ORCID:0000000207311931)

doi:10.1038/s41560-026-02040-7

DOE OSTI · 3365206

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

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Abstract

The electrochemical CO 2 reduction reaction (CO 2 RR) relies heavily on the surrounding microenvironment to promote formation of desirable multicarbon (C 2+ ) products. However, microenvironment control to achieve high C 2+ yields at industrially relevant current densities remains a crucial challenge. We report that chitosan, cellulose and chitin biopolymer coatings on CO 2 RR electrocatalysts enhance the microenvironment by increasing local CO 2 /CO concentration, reducing local water activity and providing suitable ion conductivity and local pH. This facile approach achieves C 2+ Faradaic efficiencies of 90 ± 1.7% at 1.6 A cm −2 and C 2+ 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 CO 2 RR due to excess interfacial H 2 O. These findings unveil key insights into microenvironment design to enhance C–C coupling through a simple method.

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Wei, Chaolong [Tianjin Univ. (China); National University of Singapore (Singapore)] (ORCID:0009000761505060), Yoo, Suhwan [Seoul National Univ. (Korea, Republic of)], Li, Yan [National University of Singapore (Singapore)], Ma, Haibin [National University of Singapore (Singapore)], Cheng, Yaqi [National University of Singapore (Singapore)] (ORCID:0000000307125984), Wu, Yao [National University of Singapore (Singapore)] (ORCID:0009000514237097), Sun, Guangxin [Tianjin Univ. (China); National University of Singapore (Singapore)], Zhang, Caiwei [National University of Singapore (Singapore)], He, Qian [National University of Singapore (Singapore)] (ORCID:0000000348913581), Lin, Tiras Y. [Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Computational Engineering Division] (ORCID:0000000233779933), Yeo, Boon Siang [National University of Singapore (Singapore)] (ORCID:0000000316090867), Varley, Joel B. [Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Materials Science Division; Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF)], Hwang, Yun Jeong [Seoul National Univ. (Korea, Republic of)] (ORCID:0000000209801758), He, Chunnian [Tianjin Univ. (China)] (ORCID:0000000257686598), Wong, Andrew Barnabas [National University of Singapore (Singapore)] (ORCID:0000000207311931). 2026-04-17. A scalable, biopolymer-based microenvironment for electrochemical CO 2 conversion to multicarbon products with current densities over 2 A cm −2. https://doi.org/10.1038/s41560-026-02040-7

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