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Asymmetric Electronic Modulation Accelerating Proton-Coupled Electron Transfer and CO2 Reduction at Strongly Negative
Ruina Li1, Haoyu Long1, Guoen Tang1
1Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, P. R. China.
An asymmetric Ni-Fe dual-atom electrocatalyst boosts carbon dioxide reduction to CO. It overcomes proton-electron imbalance, maintaining high CO selectivity even at negative potentials.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Electrochemical CO2 reduction is key for sustainability but faces challenges.
- Proton-electron imbalance and hydrogen evolution reaction (HER) limit selectivity at negative potentials.
Purpose of the Study:
- To develop an electrocatalyst that enhances proton-coupled electron transfer (PCET) for efficient CO2 reduction.
- To address the HER dominance and improve CO2 reduction selectivity.
Main Methods:
- Designed an asymmetric Ni-Fe dual-atom electrocatalyst.
- Investigated cross-site synergy between Ni and Fe atoms.
- Analyzed electronic modulation and interfacial proton dynamics.
Main Results:
- The Ni-Fe catalyst achieved over 95% CO selectivity across a wide potential window (-0.9 to -1.4 V).
- Demonstrated sustained CO2-to-CO conversion under deeply cathodic conditions.
- Showcased asymmetric electronic modulation to resolve PCET-HER selectivity conflict.
Conclusions:
- Asymmetric electronic modulation is an effective strategy for CO2 reduction.
- The Ni-Fe dual-atom electrocatalyst offers a promising pathway for carbon neutrality.
- This approach resolves the intrinsic PCET-HER selectivity conflict in CO2 reduction.
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