Engineering Single-Atom Active Sites on Covalent Organic Frameworks for Boosting COPhotoreduction

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

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Author(s)

  • Lei Ran
  • Zhuwei Li
  • Bei Ran
  • Jiaqi Cao
  • Yue Zhao
  • Teng Shao
  • Yurou Song
  • Licheng Sun
  • Jungang Hou

Detail(s)

Original languageEnglish
Pages (from-to)17097–17109
Journal / PublicationJournal of the American Chemical Society
Volume144
Issue number37
Online published6 Sep 2022
Publication statusPublished - 21 Sep 2022

Abstract

Solar carbon dioxide (CO2) conversion is an emerging solution to meet the challenges of sustainable energy systems and environmental/climate concerns. However, the construction of isolated active sites not only influences catalytic activity but also limits the understanding of the structure-catalyst relationship of CO2 reduction. Herein, we develop a universal synthetic protocol to fabricate different single-atom metal sites (e.g., Fe, Co, Ni, Zn, Cu, Mn, and Ru) anchored on the triazine-based covalent organic framework (SAS/Tr-COF) backbone with the bridging structure of metal-nitrogen-chlorine for high-performance catalytic CO2 reduction. Remarkably, the as-synthesized Fe SAS/Tr-COF as a representative catalyst achieved an impressive CO generation rate as high as 980.3 μmol g-1 h-1 and a selectivity of 96.4%, over approximately 26 times higher than that of the pristine Tr-COF under visible light irradiation. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to the synergic effect of atomically dispersed metal sites and Tr-COF host, decreasing the reaction energy barriers for the formation of *COOH intermediates and promoting CO2 adsorption and activation as well as CO desorption. This work not only affords rational design of state-of-the-art catalysts at the molecular level but also provides in-depth insights for efficient CO2 conversion.

Citation Format(s)

Engineering Single-Atom Active Sites on Covalent Organic Frameworks for Boosting COPhotoreduction. / Ran, Lei; Li, Zhuwei; Ran, Bei et al.

In: Journal of the American Chemical Society, Vol. 144, No. 37, 21.09.2022, p. 17097–17109.

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