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Operando nuclear magnetic resonance decodes alkali-tuned proton-electron relay boosting CO2-to-formate conversion
Yingli Shi1, Ying Liu2, Hongchun Dong1
1Physics Department & Shanghai Key Laboratory of Magnetic Resonance, School of Physics, Institute of Magnetic Resonance and Molecular Imaging in Medicine, East China Normal University, Shanghai, PR China.
Nature Communications
|January 19, 2026
Summary
Lithium doping in bismuth oxycarbonate enhances carbon dioxide electroreduction to formate by optimizing proton-coupled electron transfer (PCET) kinetics at bismuth sites. This structural modification boosts catalytic efficiency for CO2 conversion.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Proton-coupled electron transfer (PCET) kinetics are crucial for efficient CO2 electroreduction to formate.
- Understanding how trace dopants modify catalytic sites is essential for improving reaction pathways.
Purpose of the Study:
- To investigate the effect of lithium (Li) doping on bismuth oxycarbonate (BOC) for CO2 electroreduction.
- To elucidate the mechanism by which Li doping optimizes PCET kinetics at bismuth-active sites.
Main Methods:
- Operando dual-isotope (2H/13C) nuclear magnetic resonance (NMR) spectroscopy.
- Kinetic isotope effect, Tafel analysis, and in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (SEIRAS).
- Density functional theory (DFT) calculations.
Main Results:
- Li doping in BOC (BOC-Li) induces structural changes that optimize PCET.
- A more efficient proton-electron transfer pathway was observed in BOC-Li.
- DFT calculations indicate enhanced activity of Bi sites and improved adsorption of H2O/CO2.
Conclusions:
- Alkali metal doping, specifically Li, is a viable strategy for enhancing CO2 electroreduction efficiency.
- Structural engineering of catalytic sites through doping can significantly improve PCET kinetics.
- This work provides insights into optimizing electrocatalysts for CO2 conversion.
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