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Nitrogen Vacancy Induced Coordinative Reconstruction of Single-Atom Ni Catalyst for Efficient Electrochemical CO2 Reduction

journal contribution
posted on 2023-02-20, 05:17 authored by C Jia, S Li, Y Zhao, RK Hocking, W Ren, X Chen, Z Su, W Yang, Y Wang, S Zheng, F Pan, C Zhao
Transition metal nitrogen carbon based single-atom catalysts (SACs) have exhibited superior activity and selectivity for CO2 electroreduction to CO. A favorable local nitrogen coordination environment is key to construct efficient metal-N moieties. Here, a facile plasma-assisted and nitrogen vacancy (NV) induced coordinative reconstruction strategy is reported for this purpose. Under continuous plasma striking, the preformed pentagon pyrrolic N-defects around Ni sites can be transformed to a stable pyridinic N dominant Ni-N2 coordination structure with promoted kinetics toward the CO2-to-CO conversion. Both the CO selectivity and productivity increase markedly after the reconstruction, reaching a high CO Faradaic efficiency of 96% at mild overpotential of 590 mV and a large CO current density of 33 mA cm-2 at 890 mV. X-ray adsorption spectroscopy and density functional theory (DFT) calculations reveal this defective local N environment decreases the restraint on central Ni atoms and provides enough space to facilitate the adsorption and activation of CO2 molecule, leading to a reduced energy barrier for CO2 reduction.

History

Journal

Advanced Functional Materials

Volume

31

Pagination

2107072-2107072

ISSN

1616-301X

eISSN

1616-3028

Language

en

Issue

51

Publisher

Wiley

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