Coupling [Bmim]PF₆ and Pd NPs Modulated MOF-Based Material for Synergetic Regulating Electrocatalytic CO₂ Reduction.

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Metal-organic frameworks (MOFs) offer high porosity and active sites beneficial for CO₂ electroreduction reaction (CO₂RR).
• However, MOFs often suffer from low conductivity and efficiency, limiting their practical application.
• Improving selectivity and electron transfer is crucial for efficient CO₂ conversion.

Purpose of the Study:

• To design and synthesize a novel MOF-based catalyst for enhanced CO₂ electroreduction.
• To improve the selectivity and efficiency of CO₂ to CO conversion.
• To investigate the catalytic mechanism using experimental and computational methods.

Main Methods:

• Incorporation of ionic liquids (ILs) and Palladium (Pd) into Cu-BTC MOF structure.
• Electrochemical characterization including current density and Faraday efficiency (FE) measurements.
• Density Functional Theory (DFT) calculations to analyze reaction intermediates and energy barriers.

Main Results:

• The synthesized Pd-[Bmim]PF₆/Cu-BTC catalyst demonstrated exceptional selectivity for C₁ products.
• Achieved a high overall Faraday efficiency (FE) of 99.36% for C₁ products, with 93.18% FE for CO at -1.1 V_RHE.
• DFT calculations revealed a reduced free energy barrier (0.12 eV) for the *HOCO intermediate, facilitating CO desorption.

Conclusions:

• The novel Pd-[Bmim]PF₆/Cu-BTC catalyst significantly enhances CO₂ electroreduction efficiency and selectivity.
• The strategy of introducing ILs and specific metal atoms into MOFs is effective for improving catalytic performance.
• This work provides valuable insights for developing advanced MOF-based electrocatalysts for CO₂ conversion.