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Switching CO2 Electroreduction Pathways via Polyvinylpyrrolidone-Mediated Water Configuration Control
Yaoyu Yin1,2, Zhongnan Ling1, Keke Chai2,3
1Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China, 100049.
Adding trace amounts of polyvinylpyrrolidone (PVP) to electrolytes precisely controls CO2 electroreduction products. This method tunes the water configuration, selectively producing methane or multicarbon products with high efficiency.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
Background:
- Controlling the water configuration is crucial for steering CO2 electroreduction pathways.
- Achieving precise control over water arrangement at the electrode surface is a significant challenge in electrocatalysis.
Purpose of the Study:
- To demonstrate targeted control over CO2 electroreduction product distribution by adjusting polyvinylpyrrolidone (PVP) concentration.
- To investigate the role of PVP in modifying water configuration and its impact on electrocatalytic pathways.
Main Methods:
- Utilizing a Cu19CeOx electrode in 3 M KCl with varying concentrations of PVP.
- Employing electrochemical measurements to analyze product distribution and Faradaic efficiency (FE) at different current densities.
- Conducting mechanistic studies to understand the role of PVP in water configuration and intermediate adsorption.
Main Results:
- In the absence of PVP, multicarbon (C2+) products dominated CO2 electroreduction.
- Addition of 25 ppm PVP shifted the primary product to methane (CH4) with 60.4% FE at 500 mA cm-2.
- Increasing PVP to 125 ppm favored C2+ products with 90.8% FE at 800 mA cm-2.
- This approach showed universality across various copper-based catalysts.
Conclusions:
- Trace amounts of PVP can precisely control CO2 electroreduction product selectivity by altering water configuration.
- PVP modulates CO intermediate adsorption and water dissociation kinetics, dictating the reaction pathway.
- This strategy offers a versatile method for tuning electrocatalytic CO2 conversion.
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