Wang, N., Feng, H., Yang, J., Zheng, J., Zhang, Y., Hadjichristidis, N., & Li, Z. (2025). In Situ High Selectivity Contact‐Electroreduction of CO2 to Methanol Using an Imine‐Mediated Metal‐Free Vitrimer Catalyst. Angewandte Chemie International Edition, 64(19). Portico. https://doi.org/10.1002/anie.202500222
Abstract:
Metal catalysts for the CO2 reduction reaction (CO2RR) face challenges such as high cost, limited durability, and environmental impact. Although various structurally diverse and functional metal‐free catalysts have been developed, they often suffer from slow kinetics, low selectivity, and nonrecyclability, significantly limiting their practical applications. In this study, we introduce a recyclable nonmetallic polymer material (vitrimer) as a catalyst for a new platform in contact‐electrocatalysis. This approach harnesses the contact charges generated between water droplets and vitrimer to drive CO2RR, achieving methanol selectivity exceeding 90%. The imine groups within the vitrimer play a dual role, facilitating CO2 adsorption and enriching friction‐generated electrons, thereby mediating efficient electron transfer between the imine groups and CO2 to promote CO2RR. After 84 h of CO2RR, the system achieved a methanol production rate of 13 nmol·h−1, demonstrating the excellent stability of the method. Moreover, the vitrimer retains its high‐performance electrocatalytic activity even after recycling. Mechanistic studies reveal that, compared to traditional metal catalysts, the N─O bond in the imine, which adsorbs the key intermediate *OCH3, breaks more readily to produce methanol, resulting in enhanced product selectivity and yield. This efficient and environmentally friendly contact‐electroreduction strategy for CO2 offers a promising pathway toward a circular carbon economy by leveraging natural water droplet‐based contact‐electrochemistry.
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Funding Info:
This research / project is supported by the Agency for Science, Technology and Research - RIE2025 Manufacturing, Trade and Connectivity Programmatic Funding
Grant Reference no. : M22K9b0049
This research / project is supported by the Agency for Science, Technology and Research, and Italy-Singapore Science and Technology Cooperation - EURIPIDES
Grant Reference no. : R23I0IR040
This research / project is supported by the Agency for Science, Technology and Research - Science and Engineering Research Council (SERC) - Central Research Fund Use-inspired Basic Research
Grant Reference no. :
Description:
This is the peer reviewed version of the following article: Wang, N., Feng, H., Yang, J., Zheng, J., Zhang, Y., Hadjichristidis, N., & Li, Z. (2025). In Situ High Selectivity Contact‐Electroreduction of CO2 to Methanol Using an Imine‐Mediated Metal‐Free Vitrimer Catalyst. Angewandte Chemie International Edition, 64(19). Portico, which has been published in final form at https://doi.org/10.1002/anie.202500222. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.