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Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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Isomerism in Complexes
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Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction.

Yuzhu Zhou1, Quan Zhou1, Hengjie Liu1

  • 1National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, 230029, China.

Nature Communications
|June 24, 2023
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Summary

This study introduces a novel nickel single-atom catalyst for efficient carbon dioxide (CO2) reduction to carbon monoxide (CO). The catalyst demonstrates high selectivity and activity, offering insights into the mechanism of CO2 electroreduction.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Developing efficient electrocatalysts for carbon dioxide (CO2) reduction is critical for sustainable energy solutions.
  • Current catalysts often lack the required selectivity, activity, or stability for practical CO2 electroreduction.

Purpose of the Study:

  • To design and synthesize a highly efficient and selective electrocatalyst for CO2 reduction to CO.
  • To investigate the catalytic mechanism of the developed electrocatalyst.

Main Methods:

  • Synthesis of a nickel single-atom catalyst coordinated with pyrrolic and pyridinic nitrogen.
  • Electrochemical evaluation using flow cell experiments.
  • In-situ characterization using synchrotron-based infrared and X-ray absorption spectroscopy.
  • Theoretical calculations.

Main Results:

  • The Ni single-atom catalyst achieved a CO partial current density of 20.1 mA cm-2 at -0.15 V vs. RHE.
  • High turnover frequency over 274,000 h-1 at -1.0 V vs. RHE was observed.
  • Excellent Faradaic efficiency for CO (FE_CO > 90%) was maintained over a wide potential range (-0.15 to -0.9 V vs. RHE).

Conclusions:

  • The Ni single-atom catalyst exhibits superior performance for CO2 electroreduction to CO.
  • The catalytic activity originates from mono CO-adsorbed Ni single sites that balance intermediate formation and CO desorption.
  • This work provides a promising catalyst and mechanistic understanding for CO2 conversion.