Ultra-small Cu nanoparticles embedded in N-doped carbon arrays for electrocatalytic CO2 reduction reaction in dimethylformamide

作者：Zhang Xiaolong; Zhang Ying; Li Fengwang; Easton Christopher D; Bond Alan M; Zhang Jie^*

来源：Nano Research, 2018, 11(7): 3678-3690.

DOI：10.1007/s12274-017-1936-1

• copper tetracyanoquinodimethane (CuTCNQ)
• copper
• carbon arrays
• CO2 reduction
• electrocatalysis

The development of heterogeneous catalysts with a well-defined micro structure to promote their activity and stability for electrocatalytic CO2 reduction has been shown to be a promising strategy. In this work, Cu nanoparticles (similar to 4 nm in diameter) embedded in N-doped carbon (Cu@NC) arrays were fabricated by thermal decomposition of copper tetracyanoquinodimethane (CuTCNQ) under N-2. Compared to polycrystalline copper electrodes, the Cu@NC arrays provide a significantly improved number of catalytically active sites. This resulted in a 0.7 V positive shift in onset potential, producing a catalytic current density an order magnitude larger at a potential of -2.7 V vs. Fc/Fc(+) (Fc = ferrocene) in dimethylformamide (DMF). By controlling the water content in the DMF solvent, the CO2 reduction product distribution can be tuned. Under optimal conditions (0.5 vol% water), 64% HCOO-, 20% CO, and 13% H-2 were obtained. The Cu@NC arrays exhibited excellent catalytic stability with only a 0.5% decrease in the steady-state catalytic current during 6 h of electrolysis. The three-dimensional (3D) array structure of the Cu@NC was demonstrated to be effective for improving the catalytic activity of copper based catalysts while maintaining long-term catalytic stability.

• 出版日期2018-7
• 单位CSIRO