Highly efficient electroconversion of carbon dioxide into hydrocarbons by cathodized copper-organic frameworks

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Developing efficient electrocatalysts for carbon dioxide (CO2) conversion into hydrocarbons is crucial but challenging.
• Metal-biomolecule frameworks offer potential as catalytic platforms due to their tunable structures.

Purpose of the Study:

• To employ CuII/adeninato/carboxylato metal-biomolecule frameworks (CuII/ade-MOFs) for efficient electrochemical CO2 conversion into hydrocarbons.
• To investigate the catalytic performance and mechanism of these novel MOFs.

Main Methods:

• Electrochemical CO2 reduction using cathodized CuII/ade-MOF nanosheets.
• Characterization of catalytic performance, including faradaic efficiency (FE) and current density for hydrocarbon products.
• Analysis of catalyst reconstruction and active species formation.

Main Results:

• CuII/ade-MOFs exhibited excellent catalytic performance for CO2 electro-conversion, achieving a total hydrocarbon FE exceeding 73%.
• High selectivity for ethylene (C2H4) with a maximum FE of 45% at -1.4 V vs. RHE and methane (CH4) with a FE of 50% at -1.6 V vs. RHE were observed.
• Catalyst reconstruction and the formation of nitrogen-ligand-functionalized Cu nanoparticles were identified as key factors.

Conclusions:

• Cathodized CuII/ade-MOF nanosheets are effective electrocatalysts for CO2 conversion to hydrocarbons.
• The study provides insights into catalyst design for efficient CO2 electroreduction, highlighting the role of MOF reconstruction and active copper species.