Customizing Ionic Liquids Functionalized MOFs Composites with Hydrophobic Interface for Electrochemical CO₂...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical carbon dioxide reduction (CO2RR) is crucial for carbon cycle closure, producing valuable chemical feedstocks like carbon monoxide (CO).
• Developing efficient catalysts with high CO2 adsorption and selectivity remains a key challenge in CO2RR technology.

Purpose of the Study:

• To design and synthesize an ionic liquid (IL)-functionalized metal-organic framework (MOF)-based catalyst for enhanced CO2RR.
• To investigate the catalytic performance and mechanism of the modified electrocatalyst for selective CO production.

Main Methods:

• Fabrication of a Cu2O-HKUST-1/IL1/PTFE electrocatalyst by functionalizing Cu-based MOFs with ILs and PTFE.
• Electrochemical characterization, including cyclic voltammetry and chronoamperometry, to evaluate CO2RR performance.
• Density Functional Theory (DFT) calculations to elucidate reaction mechanisms and intermediate interactions.

Main Results:

• The Cu2O-HKUST-1/IL1/PTFE catalyst demonstrated high specific surface area, CO2 adsorption capacity, and charge transfer rates.
• The catalyst achieved a high C1 Faraday efficiency (FE) of 96.5%, with a specific FE for CO (FE_CO) of 92.7% at -1.7 V vs RHE.
• DFT calculations confirmed the role of ILs in promoting proton migration and CO selectivity, while PTFE suppressed hydrogen evolution.

Conclusions:

• The developed IL-functionalized MOF-based catalyst effectively enhances CO2 electroreduction to CO.
• The synergistic effect of ILs and PTFE creates an optimal hydrophobic interface for efficient CO2RR.
• This work presents a promising strategy for designing advanced electrocatalysts for CO2 conversion into valuable C1 products.