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Journal Article

Regulating electron transfer over asymmetric low-spin Co(II) for highly selective electrocatalysis


Huang,  Xing
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Wu, K.-H., Liu, Y., Tan, X., Liu, Y., Lin, Y., Huang, X., et al. (2022). Regulating electron transfer over asymmetric low-spin Co(II) for highly selective electrocatalysis. Chem Catalysis, 2(2), 372-385. doi:10.1016/j.checat.2021.12.005.

Cite as: https://hdl.handle.net/21.11116/0000-000A-28BD-5
The majority of energy conversion processes such as hydrogen peroxide production, nitrogen fixation, and CO2 reduction generally involve multi-electron transfer, resulting in multiple by-products and requiring tedious purification process. The development of highly selective electrocatalysts can not only reduce the energy consumption in the production process but also benefit to promote their large-scale application. Here, we report an asymmetric ligand design of molecular “Venus flytrap” at atomic CoII catalysts on a heterogeneous carbon surface for oxygen electrocatalysis with controlled selectivity. Our XAFS and DFT calculations show that the strong-field ligand-induced LS CoII centers offer inimitable steric-electronic advantages in capturing O2 and the capability to regulate reaction pathways through an H-bonding interaction between the ligands and peroxo intermediate. The proposed concept completes the picture of designer single-atom catalyst by covering the often overlooked exterior coordination sites, and is expected to be generally applicable to other heterogeneous catalyst systems.