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

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

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

Detail(s)

Original languageEnglish
Article numbere202219241
Journal / PublicationAngewandte Chemie - International Edition
Volume62
Issue number23
Online published5 Apr 2023
Publication statusPublished - 5 Jun 2023

Abstract

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. © 2023 Wiley-VCH GmbH.

Research Area(s)

  • Bottom-up Method, Co-N4 Sites, CO2 Reduction, MEA Device, Porphyrin Porous Organic Layers

Citation Format(s)

Exclusive Co-N4 Sites Confined in Two-dimensional Metal-Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial-Level Current. / Zhang, Wenjun; Liu, Shanshan; Yang, Yue et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 23, e202219241, 05.06.2023.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review