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Updated: Sep 30, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Vibronic Coupling of Adjacent Single-Atom Co and Zn Sites for Bifunctional Electrocatalysis of Oxygen Reduction and
Yu Yan1, Xiaonan Zheng1, Xiaoxiao Li1
1MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150080, China.
Abstract:
With the goal of improving the activity of single-atom catalysts, in-depth investigations were performed to design adjacent single-metal sites to produce a modulation effect by using symmetry breaking as an indicator of tuning the electronic structure. A CoN4-ZnN4/C catalyst composed of adjacent Co and Zn sites anchored on nitrogen-doped graphene was predicted by first-principle calculations to exhibit promising bifunctional electrocatalytic activity for oxygen reduction and evolution reactions with an overpotential of 0.225 and 0.264 V, respectively, which is superior to CoN4/C catalysts and outperforms commercial Pt/C and IrO2 benchmarks. The impressive catalytic activity originates from the remarkable asymmetric deformation and strong pseudo-Jahn-Teller vibronic coupling effect, through which the Zn site acts as a modulator to induce the symmetry-breaking phenomenon and tune the d-band structure and binding strength between key intermediates and the Co site. It provides mechanism-based insight for applying diatomic site catalysts for catalytic reactions and further understanding of the modulation effect.
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