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Updated: Jun 13, 2025
10:57
Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
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Modulating Spin State of Ni Single Atomic Center for High-Performance Electrocatalytic Carbon Dioxide Reduction
Shuang-Quan Zang1, Zhen Chen1, Jiankang Liu1
1Henan Institute of Advanced Technology, State Key Laboratory of Coking Coal Resources Green Exploitation, and College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.
Angewandte Chemie (International Ed. in English)
|June 11, 2025
Summary
Single atom catalysts with pyridinic-nitrogen coordination enable high-spin states for efficient carbon dioxide reduction, achieving excellent performance across various electrolytes and conditions.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Single atom catalysts (SACs) are promising for CO2 reduction.
- The influence of nitrogen coordination on SAC spin states and activity is underexplored.
Purpose of the Study:
- To investigate the effect of pyridinic-N vs. pyrrolic-N coordination on Ni SACs.
- To correlate spin state with electrocatalytic CO2 reduction performance.
Main Methods:
- Rapid joule-heating synthesis of Ni SACs with controlled nitrogen coordination.
- Magnetic susceptibility measurements to determine spin states.
- Electrochemical testing in H-cells and gas-diffusion flow cells.
- Theoretical calculations (DFT).
Main Results:
- Pyridinic-N coordination induces a high-spin state in Ni, while pyrrolic-N leads to a low-spin state.
- High-spin Ni-Npyridinic-C achieved 98.8% CO Faradaic efficiency and >99% at industrial current densities.
- Demonstrated excellent performance in alkaline, neutral, and acidic electrolytes, and in a zinc-CO2 battery.
Conclusions:
- Spin-state engineering via nitrogen coordination is a viable strategy for enhancing SACs.
- High-spin Ni-Npyridinic-C is a highly efficient electrocatalyst for CO2 reduction.
- This work advances scalable electrocatalyst design for efficient carbon cycling.
Keywords:
CO2 reductionCoordination structureElectrocatalysisSingle atom catalystSpin state modulationMore Related Videos
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