Dual‐Atom Catalysts Derived from a Preorganized Covalent Organic Framework for Enhanced Electrochemical Oxygen Reduction

Abstract Dual‐atom catalysts (DAC) are deemed as promising electrocatalysts due to the abundant active sites and adjustable electronic structure, but the fabrication of well‐defined DAC is still full of challenges. Herein, bonded Fe dual‐atom catalysts (Fe 2 DAC) with Fe 2 N 6 C 8 O 2 configuration were developed through one‐step carbonization of a preorganized covalent organic framework with bimetallic Fe chelation sites (Fe 2 COF). The transition from Fe 2 COF to Fe 2 DAC involved the dissociation of the nanoparticles and the capture of atoms by carbon defects. Benefitting from the optimized d ‐band center and enhanced adsorption of OOH* intermediates, Fe 2 DAC exhibited outstanding oxygen reduction activity with a half‐wave potential of 0.898 V vs. RHE. This work will guide more fabrication of dual‐atom and even cluster catalysts from preorganized COF in the future.