Yi Zeng, Hu Yuan, Yuan Wang, Shun Lu, Mohamed N. Khalil, Saddick Donkor, Donna Cairns, Xueqiang Qi, Ben Bin Xu, Qingsong Hua
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引用次数: 0
Abstract
Substituting the kinetically sluggish oxygen evolution reaction with the thermodynamically favorable urea oxidation reaction (UOR) offers a compelling strategy for simultaneously achieving energy-efficient hydrogen production and wastewater remediation. Nevertheless, the design of UOR catalysts that combine high activity with long-term durability remains a significant challenge. Herein, we report the scalable fabrication of binder-free Ni–W nanostructures directly grown on carbon paper through a controlled potentiostatic electrodeposition approach. Electrochemical kinetic analysis confirms that the electrocrystallization follows a diffusion-controlled pathway characterized by instantaneous nucleation and subsequent three-dimensional growth. The optimized Ni–W electrode delivers outstanding UOR activity, reaching a current density of 100 mA cm−2 at a potential of just 1.77 V versus the reversible hydrogen electrode. In a two-electrode urea electrolyzer configuration, the system achieves 10 mA cm−2 at only 1.54 V, markedly lower than the voltage required for conventional water splitting. Beyond the energy-efficient hydrogen generation, the system demonstrates meaningful environmental remediation capability, degrading 47% of urea over 30 h of continuous electrolysis. By integrating pollutant removal with electrolytic H2 production within a single platform, this work establishes a scalable, binder-free catalyst architecture aligned with circular economy principles and advances the frontier of sustainable energy conversion.
用热力学有利的尿素氧化反应(UOR)取代动力学缓慢的析氧反应为同时实现节能制氢和废水修复提供了一个令人信服的策略。然而,设计既具有高活性又具有长期耐用性的UOR催化剂仍然是一个重大挑战。在此,我们报告了通过可控恒电位电沉积方法直接在碳纸上生长无粘结剂的Ni-W纳米结构的可扩展制造。电化学动力学分析证实了电结晶遵循扩散控制的途径,其特征是瞬时成核和随后的三维生长。与可逆氢电极相比,优化后的Ni-W电极具有出色的UOR活性,在1.77 V的电位下达到100 mA cm - 2的电流密度。在双电极尿素电解槽配置中,系统在仅1.54 V的电压下达到10 mA cm - 2,明显低于传统水分解所需的电压。除了节能制氢之外,该系统还显示出有意义的环境修复能力,在30小时的连续电解中降解了47%的尿素。通过将污染物去除与电解制氢结合在一个单一的平台上,这项工作建立了一个可扩展的、无粘合剂的催化剂架构,符合循环经济原则,并推进了可持续能源转换的前沿。