Experimental and Computational Studies on Copper-Cerium Catalysts Supported on Nitrogen-Doped Porous Carbon for Preferential Oxidation of CO

Copper-containing cerium oxides are versatile and robust catalysts, holding great promise for future market breakthroughs for preferential oxidation of CO in the applications of fuel cells. Carbon supports could improve dispersion, redox properties, and geometric and electronic interactions of the mixed oxides for the goals of low-temperature activity and stability. We synthesized a series of CuCe catalysts supported on the nitrogen-doped porous carbon supports for experimental analyses. The experimental results and DFT calculations show that there is geometric interaction between copper and ceria species because of Cu ions into CeO2 lattice. The primary type of N element in NC support synthesized by ZIF-8 template is pyridine nitrogen, which facilitates the adsorption and activation of oxygen. The high calcination temperature facilitates the reduction of copper oxide and leads to the enrichment of copper on the oxides surface. The CuCe/NC-400 catalyst shows optimal catalytic performance due to geometric characteristics of the higher content of finely dispersed copper species and pyridine nitrogen as well as higher concentration of Ce3+ and oxygen vacancies, which together improves synergistic effect between Cu2+/Cu+ and Ce4+/Ce3+ couples. The CuCe/NC-400 catalyst also shows good resistance to H2O due to the addition of nitrogen-doped porous carbon.