In-situ electrochemical activation of Cu/Co(OH)2/Ti3C2(OH)X-MXene for improved hydrazine electrooxidation-assisted hydrogen generation
摘要
The development of high-performance hydrazine electrooxidation catalysts is crucial for reducing energy consumption in hydrogen production. In this work, a novel Cu/Co(OH)2/Ti3C2(OH)X-MXene (abbreviated as MX) catalyst was fabricated via electrodeposition, followed by surface reconstruction through an in-situ electrochemical reduction strategy. The activated catalyst, denoted as Cu/Co/Co(OH)2/MX, demonstrates remarkable performance, achieving an ultra-low overpotential of −78 mV at a current density of 10 mA cm−2, along with a small Tafel slope of 28.7 mV dec−1. Theoretical calculations reveal that the incorporation of MX significantly enhances the catalyst’s conductivity and wettability, facilitating efficient mass and electron transfer. Furthermore, MX promotes electron transfer to Co(OH)2, enabling the reduction of Co’s oxidation state and driving the electrochemical reconstruction of Co(OH)2. The addition of Cu further modulates the electronic structure by lowering the d-band center of the Co active site from −0.867 to −0.883 eV, thereby enhancing N2 desorption during hydrazine oxidation. This synergistic interplay between Cu and MX reduces the free energy barrier of the rate-determining step from 0.33 to 0.24 eV, significantly improving catalytic efficiency. As a result, a two-electrode electrolyzer incorporating this bifunctional catalyst requires only 0.252 V to achieve a current density of 100 mA cm−2, representing a voltage reduction of 1.519 V compared to conventional water electrolysis systems. These advancements highlight the catalyst’s potential for sustainable “green hydrogen” production, offering a promising avenue for energy-efficient hydrogen generation.