The construction of crystalline-amorphous coupling structure is one of the effective strategies to enhance the performance of oxygen evolution reaction (OER) and urea oxidation reaction (UOR). Herein, NiFe-LDH/NiMoO4/NF with high oxygen evolution and urea oxidation performance was successfully prepared by electrodeposition of amorphous substances on the crystalline precursor of hydrothermal synthesis. Remarkably, the NiFe-LDH/NiMoO4/NF displays exceptional electrocatalytic performance for OER and UOR, with a potential of only 1.57 V vs. RHE at 100 mA cm−2 and the Tafel slope of 54.4 mV dec−1 for OER, high UOR activity with a potential of 1.45 mV@100 mA cm−2 and the Tafel slope of 20.4 mV dec−1 in 1.0 M KOH with 0.33 M urea solution. In a hybrid acid-base electrolysis system for urea oxidation-assisted H2 production using NiFe-LDH/NiMoO4/NF as the anode electrode and Pt/C/NF as the cathode electrode, the process requires a cell voltage of only 0.55 V vs. RHE at 10 mA cm−2. Moreover, this hybrid acid/base system demonstrates stable operation for 110 h with minimal attenuation at a current density of 100 mA cm−2. These results indicate a facile strategy for the design of electrodes with crystalline-amorphous coupling structures for energy conversion.
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