Guan Zeyi, Zhang Liuyan, Xie Yiqi, Wu Danting, Yuan Binkai, Wu Lichan, Shen Gengzhe, Tan Guibin, Guo Fujian
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, PR China.
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, PR China; State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment, Guangdong University of Technology, Guangzhou 510006, PR China; Yangjiang Advanced Alloys Laboratory, Yangjiang 529500, Guangdong, China.
J Colloid Interface Sci. 2025 Sep 16;702(Pt 2):139037. doi: 10.1016/j.jcis.2025.139037.
Alkaline water electrolysis is recognized as an environmentally sustainable approach for generating high-energy-density clean hydrogen. However, its efficiency remains largely limited by the sluggish kinetics water dissociation in the hydrogen evolution reaction (HER), the challenge of activating water molecules, and the excessive consumption of OH and high adsorption energy barriers of oxygenated intermediates during the oxygen evolution reaction (OER). In this work, A nanoneedle-structured Ru-NiCo₂O₄-Se electrocatalyst was developed, demonstrating excellent bifunctional electrocatalytic performance for both HER and OER. Through a combination of experimental characterizations and theoretical simulations, it had been revealed that the sharp-tip nanoneedle morphology generates intense local electric fields. These fields facilitate the enrichment of K ions at the cathode, optimized the interfacial water structure, and substantially lower the energy barrier required for water dissociation. At the anode, the tip effect facilitated OH accumulation, enhanced reactant mass transport, and accelerated OER kinetics. Moreover, metal-support interactions (MSI) between Ru nanoclusters and the support effectively modulate the adsorption behavior of H* and oxygenated intermediates, further boosting catalytic performance. The catalyst achieves overpotentials as low as -48 mV for HER and + 231 mV for OER at a current density of 10 mA·cm, and delivers a high overall water splitting current of 100 mA·cm at a cell voltage of only 1.7 V, along with remarkable long-term durability over hundreds of hours. This study presents an innovative strategy based on interfacial microenvironment engineering and electronic structure modulation, paving a fresh pathway for the development of cost-effective, high-performance, and long-lasting bifunctional electrocatalysts tailored for clean energy conversion.
碱性水电解被认为是一种环境可持续的方法，用于生产高能量密度的清洁氢气。然而，其效率在很大程度上仍受到析氢反应（HER）中水分子解离动力学缓慢、激活水分子的挑战以及析氧反应（OER）过程中OH的过度消耗和含氧中间体的高吸附能垒的限制。在这项工作中，开发了一种纳米针状结构的Ru-NiCo₂O₄-Se电催化剂，展示了对HER和OER均优异的双功能电催化性能。通过实验表征和理论模拟相结合，揭示了尖锐尖端的纳米针形态会产生强烈的局部电场。这些电场促进了阴极处K离子的富集，优化了界面水结构，并大幅降低了水分子解离所需的能垒。在阳极，尖端效应促进了OH的积累，增强了反应物的质量传输，并加速了OER动力学。此外，Ru纳米团簇与载体之间的金属-载体相互作用（MSI）有效地调节了H*和含氧中间体的吸附行为，进一步提高了催化性能。该催化剂在电流密度为10 mA·cm²时，HER的过电位低至-48 mV，OER的过电位为+231 mV，并且在仅1.7 V的电池电压下，能提供100 mA·cm²的高全水解电流，同时具有超过数百小时的显著长期耐久性。本研究提出了一种基于界面微环境工程和电子结构调制的创新策略，为开发用于清洁能源转换的经济高效、高性能和持久的双功能电催化剂开辟了一条新途径。
