用于阴离子交换膜电解水的重组金属有机框架中增强氧进化的起源

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Ying Li, Liu Yang, Xiaolei Hao, Xiaopei Xu, Lingling Xu, Prof. Bo Wei, Prof. Zhongwei Chen
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引用次数: 0

摘要

金属有机框架(MOFs)因其结构的灵活性和可调性而备受赞誉,是探索氧进化反应(OER)的重要催化剂原型。然而,它们在氧进化反应(尤其是在工业大电流环境下)中的复杂转变给准确阐明其结构与活性的相关性带来了巨大挑战。在这里,我们利用电氧化过程实现了可控的 MOF 重构,发现铁的掺杂加速了 Ni(Fe)-MOF 的结构演化,同时伴随着 Ni-O 键的伸长,并通过原位拉曼光谱和紫外可见光谱进行了监测。理论建模进一步表明,NiO6 八面体中的铁掺杂和缺陷诱导的拉伸应变增强了金属 ds-Op 杂化,优化了它们的吸附行为,提高了 OER 活性。重构的 Ni(Fe)-MOF 可作为阴离子交换膜水电解的阳极,在 2.2 V 电压下达到 3.3 A cm-2 的显著电流密度,同时在 0.5 A cm-2 到 1 A cm-2 的 160 小时内保持同样稳定的运行。这项研究提高了我们对 OER 催化剂重构的理解,为设计跨电化学平台的高效催化剂提供了前景广阔的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Origin of Enhanced Oxygen Evolution in Restructured Metal–Organic Frameworks for Anion Exchange Membrane Water Electrolysis

Origin of Enhanced Oxygen Evolution in Restructured Metal–Organic Frameworks for Anion Exchange Membrane Water Electrolysis

Metal–Organic Frameworks (MOFs), praised for structural flexibility and tunability, are prominent catalyst prototypes for exploring oxygen evolution reaction (OER). Yet, their intricate transformations under OER, especially in industrial high-current environments, pose significant challenges in accurately elucidating their structure–activity correlation. Here, we harnessed an electrooxidation process for controllable MOF reconstruction, discovering that Fe doping expedites Ni(Fe) MOF structural evolution, accompanied by the elongation of Ni−O bonds, monitored by in situ Raman and UV/Visible spectroscopy. Theoretical modeling further reveals that Fe doping and defect-induced tensile strain in the NiO6 octahedra augments the metal ds-O p hybridization, optimizing their adsorption behavior and augmenting OER activity. The reconstructed Ni(Fe) MOF, serving as the anode in anion exchange membrane water electrolysis, achieves a noteworthy current density of 3300 mA cm−2 at 2.2 V while maintaining equally stable operation 500 mA cm−2 for 300 h and 1000 mA cm−2 for 170 h. This undertaking elevates our comprehension of OER catalyst reconstruction, furnishing promising avenues for designing highly efficacious catalysts across electrochemical platforms.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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