Abstract
Electrocatalytic urea oxidation reaction (UOR) is a prospective method to substitute the slow oxygen evolution reaction (OER) and solve the problem of urea-rich water pollution due to the low thermodynamic voltage, but its complex six-electron oxidation process greatly impedes the overall efficiency of electrolysis. Here, density functional theory (DFT) calculations imply that the metallic Ni3S2 and semiconductive MoS2 could form Mott-Schottky catalyst because of the suitable band structure. Therefore, we synthesized MoS2/Ni3S2 electrocatalyst by a simple hydrothermal method, and studied its UOR and hydrogen evolution reaction (HER) performance. The formed MoS2/Ni3S2 Schottky heterojunction is only required 109 and 166 mV to obtain ±10 mA cm−2 for UOR and HER, respectively, showing great bifunctional catalytic activity. Moreover, the full urea electrolysis driven by MoS2/Ni3S2 delivers 10 and 100 mA cm−2 at a relatively low potential of 1.44 and 1.59 V. Comprehensive experiments and DFT calculations demonstrate that the MoS2/Ni3S2 Schottky heterojunction causes self-driven charge transfer at the interface and forms built-in electric field, which is not only benefit to reduce H* adsorption energy, but also helps to adjust the absorption and directional distribution of urea molecules, thereby promoting the activity of decomposition of water and urea. This research furnishes a tactic to devise more efficient catalysts for H2 generation and the treatment of urea-rich water pollution.
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