Exclusive Co-N4 Sites Confined in Two-dimensional Metal-Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial-Level Current

Exclusive Co-N4 Sites Confined in Two-dimensional Metal-Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial-Level Current

Angewandte Chemie International Edition

10.1002/anie.202219241

https://doi.org/10.1002/anie.202219241

Wenjun Zhang, Shanshan Liu, Yue Yang, Haifeng Qi, Shibo Xi, Yanping Wei, Jie Ding, Zhu‐Jun Wang, Qunxiang Li, Bin Liu, Zupeng Chen

05 April 2023

Zhang, W., Liu, S., Yang, Y., Qi, H., Xi, S., Wei, Y., Ding, J., Wang, Z., Li, Q., Liu, B., & Chen, Z. (2023). Exclusive Co‐N4 Sites Confined in Two‐dimensional Metal‐Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial‐Level Current. Angewandte Chemie International Edition, 62(23). Portico. https://doi.org/10.1002/anie.202219241

Metal‐organic framework catalysts bring new opportunities for CO2 electrocatalysis. Herein, we first conduct density‐functional theory calculations and predict that Co‐based porphyrin porous organic layers (Co‐PPOLs) exhibit good activity for CO2 conversion because of the low *CO adsorption energy at Co‐N4 sites, which facilitates *CO desorption and CO formation. Then, we prepare two‐dimensional Co‐PPOLs with exclusive Co‐N4 sites through a facile surfactant‐assisted bottom‐up method. The ultrathin feature ensures the exposure of catalytic centers. Together with large specific area, high electrical conductivity and CO2 adsorption capability, Co‐PPOLs achieve a peak faradaic efficiency for CO production (FECO=94.2 %) at a moderate potential in CO2 electroreduction, accompanied with good stability. Moreover, Co‐PPOLs reach an industrial‐level current above 200 mA in a membrane electrode assembly reactor, and maintain near‐unity CO selectivity (FECO>90 %) over 20 h in CO2 electrolysis.

Publisher Copyright

This research / project is supported by the Agency for Science, Technology and Research (A*STAR) - Low Carbon Energy Research Finding Initiative (LCERFI01-0033 | U2102d2006)
Grant Reference no. : U2102d2006

This is the peer reviewed version of the following article: Zhang, W., Liu, S., Yang, Y., Qi, H., Xi, S., Wei, Y., Ding, J., Wang, Z., Li, Q., Liu, B., & Chen, Z. (2023). Exclusive Co‐N4 Sites Confined in Two‐dimensional Metal‐Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial‐Level Current. Angewandte Chemie International Edition, 62(23). Portico, which has been published in final form at https://doi.org/10.1002/anie.202219241. 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.

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