Cation Enrichment Promotes High-rate CO Electroreduction to C₂₊ Liquid Products

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical reduction of CO2 to multicarbon (C2+) liquids is vital for CO2 emission reduction and clean energy solutions.
• Achieving high efficiency and selectivity in CO2 electroreduction remains a significant challenge.

Purpose of the Study:

• To develop a novel surface-modification strategy for copper-based catalysts to enhance CO2 electroreduction.
• To improve the efficiency and selectivity of C2+ liquid product formation from CO2.

Main Methods:

• Utilized electrochemically active polymeric 1,4,5,8-naphthalenetetracarboxylic dianhydride (PNTCDA) to modify copper nanosheets (PM-Cu).
• Employed electrochemical analysis and computational simulations to investigate the catalyst's mechanism.
• Investigated the role of potassium ions (K+) in the electric double layer.

Main Results:

• The PNTCDA modification rearranged reactive species and anchored K+ ions, optimizing the local microenvironment.
• The PM-Cu catalyst demonstrated efficient dehydration of hydrated K+ and reduced active water molecules, suppressing hydrogen evolution.
• Achieved ampere-scale current densities with over 90% selectivity for C2+ liquid products.

Conclusions:

• Surface modification with electrochemically active organics can effectively modulate CO2 reduction.
• The developed catalyst shows significant potential for sustainable energy storage and industrial carbon utilization.
• This approach offers a promising pathway for efficient CO2 conversion into valuable chemicals.