articleJournal of the American Chemical SocietyJan 13, 2026Closed access

Dual-Spin Centers in a Grid-like Covalent Organic Framework Promote Near-Unity CO 2 Electroreduction

QGQianfeng GuYXYinger XinMSMingzi SunYZYuanzhang ZhaoYLYaqi Liao

City University of Hong Kong · City University of Hong Kong, Shenzhen Research Institute

PubMed
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Abstract

Spin manipulation has emerged as a promising strategy for enhancing molecular electrocatalytic performance. However, precisely controlling dual spin centers and delineating their contribution to reaction kinetics remain a considerable challenge. Herein, we demonstrate that incorporating quinone moieties into a grid-like covalent organic framework (COF) enables a dual-spin-center catalysis system, simultaneously stabilizing semiquinone radicals and inducing an electronic reconfiguration with low-spin character at the cobalt center. Spectroscopic and theoretical analyses reveal a synergistic mechanism. The spin-polarized electron density of semiquinone radicals creates an internal potential gradient that…

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Topics & keywords

Topics
Keywords
  • Semiquinone
  • Delocalized electron
  • Radical
  • Covalent bond
  • Cobalt
  • Catalysis
  • Electron paramagnetic resonance
  • Density functional theory
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