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Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
Synergistic Interaction Between N-Heterocyclic Carbene (NHC)-Anchored Cu(I) Atom and In Situ-Generated Cu
Li-Hong Jia1, Xian-Ming Zhang1,2
1College of Chemistry & Chemical Engineering, Taiyuan University of Technology, Taiyuan, People's Republic of China.
This study introduces a novel catalyst for electrochemical CO2 reduction, enhancing C2H4 production. The synergistic N-heterocyclic carbene-anchored Cu(I) and Cu nanoparticles in a MOF framework improve efficiency and selectivity.
Area of Science:
- Catalysis
- Materials Science
- Electrochemistry
Background:
- Electrochemical reduction of CO2 (eCO2RR) offers a sustainable path for CO2 mitigation and valuable chemical production.
- Challenges include high energy barriers for C-C bond formation and competing hydrogen evolution reaction (HER).
Purpose of the Study:
- To develop a synergistic catalyst for efficient eCO2RR to C2H4.
- To investigate the role of N-heterocyclic carbene (NHC) ligands in enhancing catalyst performance.
Main Methods:
- Synthesis of a MOF-808 framework incorporating NHC-anchored Cu(I) atoms and in situ generated Cu nanoparticles.
- Electrochemical characterization and experimental studies.
- Density functional theory (DFT) calculations to elucidate reaction mechanisms.
Main Results:
- Achieved high Faradaic efficiency (FE) of 61.0% for C2H4 and 79.5% for total C2+ products in neutral electrolyte.
- NHC ligand promoted proton transfer and CO hydrogenation, stabilizing key intermediates.
- Synergy between molecular NHC-Cu(I) and Cu nanoparticles suppressed HER and facilitated C-C coupling.
Conclusions:
- The NHC-Cu(I)/Cu nanoparticle catalyst in MOF-808 demonstrates superior performance for eCO2RR.
- The dual role of NHC ligands is crucial for efficient CO2 conversion.
- This work provides a design strategy for advanced MOF-based electrocatalysts.
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