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    原位重构Sr-NiFeOOH纳米片用于阴离子交换膜电解水

    In-situ Reconstructed Sr-NiFeOOH Nanosheets for Anion Exchange Membrane Water Electrolysis

    • 摘要: 阴离子交换膜电解水制氢技术由于可以使用非贵金属催化剂成为研究热点,其阳极四电子质子耦合过程表现出迟滞的反应动力学,严重阻碍了其产业化发展。本研究通过水热法制备锶(Sr)掺杂的镍铁硒化物预催化剂,在碱性析氧反应条件下原位重构得到Sr-NiFeOOH超薄纳米片。通过透射电子显微镜表征其形貌,采用X射线吸收谱探究双金属的价态及配位环境,利用线性伏安曲线、塔菲尔斜率及电化学活性面积评估其析氧反应性能。Sr-NiFeOOH超薄纳米片富含丰富的双金属空位,通过X射线吸收精细结构表征说明金属与氧的共价性增强从而激活晶格氧,同时由于双金属空位使金属与界面羟基的价电子耦合作用增强利于晶格氧重新填充,从而协同提升催化活性及稳定性。在阴离子交换膜电解水制氢中,该催化剂在2 V的槽压下能够实现2.75 A·cm−2的大电流,且在工业电流密度下稳定运行123 h,无明显衰减。因此,该催化剂具有廉价、高效且实用的工业化优势,对低碳产业化转型提供设计思路。

       

      Abstract: Anion exchange membrane water electrolysis (AEMWE) for hydrogen production has emerged as a research hotspot because it enables the use of non-noble metal catalysts. However, the anodic four-electron proton-coupled reaction exhibits sluggish kinetics, which seriously hinders its industrialization. Here, a strontium-doped nickel-iron selenide precatalyst was prepared via a hydrothermal method, and it was in-situ reconstructed into Sr-NiFeOOH ultrathin nanosheets under alkaline oxygen evolution reaction (OER) conditions. Transmission electron microscopy (TEM) was used to characterize the morphology. X-ray absorption spectroscopy (XAS) was employed to explore the valence states and coordination environments of the bimetallic sites. Linear sweep voltammetry, Tafel slope, and electrochemical active surface area were utilized to evaluate the OER catalytic performance. The Sr-NiFeOOH ultrathin nanosheets are rich in bimetallic vacancies. Extended X-ray absorption fine structure (EXAFS) results confirm the enhanced covalency of metal-oxygen bonds to activate lattice oxygen. Meanwhile, the bimetallic vacancies strengthen the valence electron coupling between metal sites and interfacial hydroxyl groups, facilitating the replenishment of lattice oxygen. These effects synergistically improve the catalytic activity and structural stability. In the AEMWE system, the catalyst delivers a large current density of 2.75 A·cm−2 at a cell voltage of 2 V, and maintains stable operation for 123 h at industrial current densities without obvious degradation. Therefore, the low-cost and high-efficiency catalyst exhibits promising practical industrial prospects and provides a rational design strategy for low-carbon industrial transformation.

       

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