Electrocatalytic reduction of CO2 to formic acid on palladium-graphene nanocomposites gas-diffusion electrode.

Abstract

Palladium-graphene nanocomposites catalysts for the conversion of CO2 to formic acid were prepared by means of sodium borohydride reduction of K2PdCl4 in a graphite oxide suspension, and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and cyclic voltammetry (CV) technologies. The characterization results showed that graphene with a d-spacing of 3.82 Å was fabricated, and palladium nanoparticles with an average size of 3.8 nm were highly dispersed in the graphene sheets with amorphous structure. The cyclic voltammogram analyses indicated palladium-graphene nanocomposites catalysts posed high catalytic activity for the CO2 reduction and the rate-determining step was the CO2 diffusion process from bulk solution to electrode surface. Then the electrocatalytic reduction of CO2 was investigated in a diaphragm electrolysis device, using Pd/graphene gas-diffusion electrode as a cathode and a Ti/RuO2 net anode. The reduction process was optimized by the application of factorial design 2(3) (voltage, reaction time and electrolyte concentration) and response surface methodology (RSM). Optimum conditions for the production of formic acid were given as following: voltage: 5.1 V, reaction time: 50.4 min and electrolyte concentration: 0.5 mol L(-1). The yield of formic acid formation was 3157.7 mg L(-1) and Faraday efficiency was 86.9% under the optimum operation condition.