Novel Gel method MXene-Supported Dual-Site PtNi-NiO for Electrocatalytic Water Reduction and Urea Oxidation

Small. 2024 Oct 31:e2409461. doi: 10.1002/smll.202409461. Online ahead of print.

Abstract

Compared to the traditional oxygen evolution reaction (OER), the urea oxidation reaction (UOR) generally exhibits a lower overpotential during the electrolytic process, which is conducive to the hydrogen evolution reaction (HER) at the cathode. The superior structure and abundant sites play a crucial role in promoting the adsorption and cleavage of urea molecules. Therefore, this paper introduces a simple metal cation-induced gelation method to prepare an electrocatalyst with PtNi alloy-NiO dual sites supported on Ti3C2Tx, which simultaneously exhibits excellent UOR and HER performance. PtNi-NiOx/Ti3C2Tx demonstrates good catalytic activity for the urea oxidation reaction, requiring only 1.364 V (overpotential of 0.994 V) to achieve a current density of 100 mA cm-2 in UOR, and also exhibits remarkable catalytic activity in the hydrogen evolution reaction, with PtNi-NiOx/Ti3C2Tx achieving a current density of 10 mA cm-2 in HER with only 24 mV of overpotential. In the UOR//HER two-electrode electrolysis cell, it requires only 1.361 and 1.538 V to reach current densities of 10 and 100 mA cm-2, respectively. According to density functional theory (DFT) calculations, the dual active sites can intelligently adsorb the electron-donating/electron-withdrawing groups in urea molecules, activate chemical bonds, and thereby initiate urea decomposition.

Keywords: HER; MXene; PtNi‐NiO; UOR; dual‐site.