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Reactant-Sustained Dynamically Stable Interfacial Hydrogen-Bond Network for Highly Selective, Ampere-Level Ethylene
Li Yuan1, He Zhang1, Xuesong Liu1
1School of Chemical Engineering, Sichuan University, Chengdu, P. R. China.
A novel metal-organic framework (MOF) electrocatalyst (Co-PET@NF) creates a unique hydrogen-bond network for efficient ethylene glycol electrooxidation (EGOR). This advanced catalyst achieves high selectivity and stability, offering a sustainable pathway for biomass upgrading.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- The catalyst-electrolyte interface is crucial for electrochemical reactions, but dynamic stability and efficient proton transfer are challenging at high current densities.
- Engineering stable interfaces for continuous reactant supply and proton-coupled electron transfer is key for advanced electrocatalysis.
Purpose of the Study:
- To develop a highly selective electrocatalyst for ethylene glycol electrooxidation (EGOR) using a metal-organic framework (MOF).
- To investigate the role of interfacial hydrogen-bond networks in enhancing catalyst activity and stability.
Main Methods:
- Fabrication of an ultrathin MOF-derived electrocatalyst (Co-PET@NF).
- Electrochemical characterization of ethylene glycol electrooxidation (EGOR) performance.
- Mechanistic studies using in-situ techniques to probe interfacial interactions and hydrogen-bond network dynamics.
Main Results:
- Co-PET@NF demonstrated high selectivity for formate production (FEFA = 92.8%) at 1.0 A cm-2 due to enhanced ethylene glycol adsorption and a stable hydrogen-bond network.
- The catalyst facilitated rapid proton transfer and maintained a localized alkaline surface microenvironment, crucial for stability.
- In a coupled system, Co-PET@NF reduced cell voltage by 260 mV at 1.0 A cm-2 compared to water electrolysis and showed stable operation for 120 h.
Conclusions:
- The reactant-enhanced hydrogen-bond network strategy is effective for stabilizing interfaces and improving selectivity in electrocatalysis.
- This MOF-based approach offers a sustainable method for biomass and plastic upgrading through efficient alcohol electrooxidation.
- The findings highlight the importance of interfacial engineering for designing next-generation electrocatalysts.
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