2D Ni-organic frameworks decorated carbon nanotubes encapsulated Ni nanoparticles for robust CN and HO bonds cleavage

In this work, we report a robust bifunctional electrocatalyst composed of 2D Ni- organic frameworks (Ni-MOF) and nitrogen doped carbon nanotubes encapsulated Ni nanoparticles (Ni-MOF@Ni-NCNT) for CN and HO bonds dissociation. Due to the presence of Ni-NCNT, adsorption of OH^- species is enhanced and CO₂ binding strength is simultaneously weakened leading to a boosted urea oxidation reaction performance reflected by decrement in potential at 100 mA cm^-2 by 69 mV. The loosened binding strength with CO₂ specie is highlighted by in-situ electrochemical impedance spectroscopy (EIS) test and DFT calculation. Moreover, the alkaline hydrogen evolution reaction (HER) performance of Ni-MOF@Ni-NCNT is better than Ni-MOF and Ni-NCNT evidenced by the overpotential at 50 mA cm^-2 decreased by 224 mV and 900 mV ascribed to the synergistic effect, in which Ni-MOF, Ni nanoparticles and Ni-Nx-C facilitates water adsorption, dissociation and adsorption/combination of hydrogen ions, respectively. The assembled HER- urea oxidation reaction (UOR) system requires only 1.33 V to reach 10 mA cm^-2, 70 mV lower than water splitting driven by Pt/C-IrO₂.