A Multiscale Strategy to Construct Cobalt Nanoparticles Confined within Hierarchical Carbon Nanofibers for Efficient...

The efficiency of CO₂ electroreduction has been largely limited by the activity of the catalysts as well as the three-phase interface. Herein, a multiscale strategy is proposed to synthesize hierarchical nanofibers covered by carbon nanotubes and embedded with cobalt nanoparticles (Co/CNT/HCNF). The confinement effect of carbon nanotubes can restrict the diameter of the cobalt particles down to several nanometers and prevent the easy corrosion of these nanoparticles. The three-dimensional carbon nanofibers, in size range of several hundred nanometers, improve the electrochemically active surface area, facilitate electron transfer, and accelerate CO₂ transportation. These cross-linked carbon nanofibers eventually form a freestanding Co/CNT/HCNF membrane of dozens of square centimeters. Consequently, Co/CNT/HCNF produces CO with 97% faradaic efficiency at only -0.4 V_RHE cathode potential in an H-type cell. From the regulation of catalyst nanostructure to the design of macrography devices, Co/CNT/HCNF membrane can be directly used as the gas-diffusion compartment in a flow cell device. Co/CNT/HCNF membrane generates CO with faradaic efficiencies higher than 90% and partial current densities greater than 300 mA cm^-2 for at least 100-h stability. This strategy provides a successful example of efficient catalysts for CO₂ electroreduction and also has the feasibility in other self-standing energy conversion devices.