Simultaneous Defect and Size Control of Metal-Organic Framework Nanostructures for Highly Efficient Carbon Dioxide Electroreduction to Multicarbon Products

Electrocatalytic carbon dioxide (CO2) reductionreaction(CO2RR) has offered a sustainable approach in convertingan anthropogenic CO2 source to chemicals and fuels to promotecarbon neutral. However, it remains challenging to prepare high-performancecatalysts for efficient and selective CO2 electroreduction,especially toward the high-vaule multicarbon products. Here we reportthe facile synthesis of four kinds of nearly monodispersed CuTrz (HTrz= 1H,1,2,4-triazole) metal-organic framework(MOF) nanostructures with different sizes by controlling the reactionkinetics. Significantly, small CuTrz nanostructures demonstrate muchsuperior CO2RR performance over the large counterpartstoward multicarbon production in neutral electrolytes, with optimizedFaradaic efficiency of 55.4% and 81.8% for ethylene and multicarbonproducts, respectively. Detailed structural characterizations revealthat small CuTrz nanostructures are polycrystalline and rich in grainboundaries, while the large ones are single crystalline. This workhighlights the importance of simultaneous defect and size controlof MOFs in boosting their CO2RR performance for multicarbonproduction.