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Temperature-Induced Low-Coordinate Ni Single-Atom Catalyst for Boosted CO2 Electroreduction Activity.

Na Wang1, Haoyue Li1, Haojing Wang2

  • 1Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, 450052, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|April 25, 2023
PubMed
Summary

A new, scalable method creates highly efficient nickel single-atom catalysts (SACs) for CO2 reduction. These catalysts show excellent performance and stability, converting CO2 to valuable products with high selectivity.

Keywords:
Ni single atomscoordination environmentselectrochemical CO 2 reductionlow-coordinate catalystsuniversality

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Single-atom catalysts (SACs) are promising for CO2 electroreduction but face challenges in scalable synthesis and structural control.
  • Existing methods for SAC preparation are often complex, expensive, and lack general applicability.
  • Tuning the coordination environment of SACs is difficult due to their inherent structural vulnerability.

Purpose of the Study:

  • To develop a simple, universal, and scalable strategy for fabricating single-atom catalysts (SACs).
  • To investigate the effect of nitrogen coordination number on the CO2 electroreduction performance of Ni SACs.
  • To achieve high efficiency and stability in converting CO2 to value-added products.

Main Methods:

  • A one-step pyrolysis method using melamine, Ni(NO3)∙6H2O, and polyvinylpyrrolidone at varying temperatures.
  • Fabrication of Ni SACs with controlled nitrogen coordination numbers.
  • Electrochemical measurements and theoretical calculations to evaluate catalytic performance and understand reaction mechanisms.

Main Results:

  • Low-coordinate Ni SACs demonstrated outstanding CO2 reduction performance, achieving 98.5% Faradaic efficiency (FECO) for CO production at -0.76 V.
  • High CO current density of 24.6 mA cm⁻² was achieved, with FECO > 91.0% across a wide potential window (-0.56 to -1.16 V).
  • The catalysts exhibited excellent stability, with no significant degradation over 50 hours of operation, attributed to their coordinatively unsaturated structure facilitating *COOH intermediate formation.

Conclusions:

  • The developed one-step pyrolysis strategy is a simple, universal, and scalable approach for synthesizing SACs.
  • Low-coordinate Ni SACs show superior activity and stability for electrochemical CO2 reduction, offering a promising pathway for CO2 valorization.
  • The method's universality was demonstrated by successfully preparing other metallic SACs.