Cui Xin, Ding Yunxuan, Tang Tang, Wang Linqin, Zhang Feiyang, Li Peifeng, Sun Licheng, Zhang Biaobiao
Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Hangzhou 310030, China.
Division of Solar Energy Conversion and Catalysis at Westlake University, Zhejiang Baima Lake Laboratory Co., Ltd., Hangzhou 310000, China.
ACS Appl Mater Interfaces. 2025 May 21;17(20):29659-29668. doi: 10.1021/acsami.5c03491. Epub 2025 May 8.
Anion-exchange membrane water electrolysis (AEM-WE) offers a promising alternative for efficient water electrolysis, providing low-cost and high-purity hydrogen production. However, the slow reaction kinetics associated with the oxygen evolution reaction (OER) continue to pose a significant obstacle. In this work, we synthesized nanometer micron hierarchical NiFeMoO as OER precatalysts, which were completely reconstructed into hierarchical NiFeOOH (NiFeOOH), demonstrating remarkable OER activity, with overpotentials of 162/245 mV required to achieve current densities of 10/1000 mA cm in 1.0 M KOH. Additionally, it demonstrated robust stability exceeding 1000 h at 1000 mA cm. Furthermore, NiFeOOH demonstrated excellent long-term stability in AEM-WE, maintaining a current density of 1000 mA cm at a cell voltage of 1.55 V (80 °C) for over 160 h and achieving a reliable performance beyond 1000 h at room temperature. analyses, including X-ray absorption fine structure (XAFS), Raman spectroscopy, and Fourier transform infrared spectroscopy (FTIR), combined with density functional theory (DFT) calculations, reveal that the OER process of NiFeOOH primarily follows an adsorption evolution mechanism (AEM) at the Ni site. Meanwhile, Fe acts as a Lewis acid, promoting Ni valence and thereby enhancing the OER performance. This study emphasized the crucial role of precatalyst engineering for efficient NiFe-based catalysts and analyzed the role of Fe in the OER catalytic cycle.
阴离子交换膜水电解（AEM-WE）为高效水电解提供了一种有前景的替代方案，可实现低成本、高纯度制氢。然而，与析氧反应（OER）相关的缓慢反应动力学仍然是一个重大障碍。在这项工作中，我们合成了纳米微米级的NiFeMoO作为OER预催化剂，其完全重构为分级结构的NiFeOOH，展现出显著的OER活性，在1.0 M KOH中达到10/1000 mA cm²的电流密度所需的过电位分别为162/245 mV。此外，在1000 mA cm²下其稳定性超过1000小时。再者，NiFeOOH在AEM-WE中表现出出色的长期稳定性，在1.55 V（80°C）的电池电压下保持1000 mA cm²的电流密度超过160小时，在室温下超过1000小时实现可靠性能。包括X射线吸收精细结构（XAFS）、拉曼光谱和傅里叶变换红外光谱（FTIR）在内的分析，结合密度泛函理论（DFT）计算，表明NiFeOOH的OER过程主要在Ni位点遵循吸附演化机制（AEM）。同时，Fe作为路易斯酸，促进Ni的价态变化，从而提高OER性能。本研究强调了预催化剂工程对高效NiFe基催化剂的关键作用，并分析了Fe在OER催化循环中的作用。
