Post-modification engineering of cerium metal-organic frameworks for efficient visible light-driven water oxidation

IF 9.6 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Rare Metals Pub Date : 2024-07-04 DOI:10.1007/s12598-024-02844-0

Lin-Zhu Zhang, Lu Chen, Gui-Yang Yan, Ruo-Wen Liang, Hong-Hui Ou

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Abstract

Metal-organic frameworks (MOFs) are highly desirable for promising photocatalytic water splitting, but their practical application is greatly limited due to their unstable chemical properties and insufficient visible light response as well as low charge-carries utilization, especially in photocatalytic O₂ production. Herein, we present a post-modification engineering to modulate cerium metal-organic frameworks (Ce-MOFs) for realizing efficient photocatalytic water oxidation to liberate O₂ by visible light. The one-step partial oxidation strategy is adopted to modify pristine Ce-MOFs, yielding the new Ce-MOFs (MV-Ce-MOFs) with mixed valence of Ce³⁺/Ce⁴⁺. Creating the Ce nodes of a mixed valence state can effectively extend the optical absorption to the visible region, expose more catalytically active sites and inhibit the recombination of photoinduced charges. Consequently, the MV-Ce-MOFs exhibit high activity for photocatalytic O₂ evolution under visible light, manifesting an impressive 1.6% apparent quantum efficiency (AQY) under monochromatic irradiation of 405 nm. The regulation engineering of MOF metal node valence heralds a new paradigm for designing MOF-based photocatalysts.

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用于可见光驱动的高效水氧化的铈金属有机框架后修饰工程

金属有机框架（MOFs）具有广阔的光催化水分离前景，但由于其化学性质不稳定、对可见光响应不足以及电荷携带利用率低等原因，其实际应用受到很大限制，尤其是在光催化产生 O2 方面。在此，我们提出了一种后修饰工程方法来调节铈金属有机框架（Ce-MOFs），以实现高效的光催化水氧化，从而在可见光下释放出 O2。该研究采用一步部分氧化策略对原始 Ce-MOFs 进行改性，得到了具有 Ce3+/Ce4+ 混合价的新 Ce-MOFs (MV-Ce-MOFs)。创建混合价态的 Ce 节点可以有效地将光吸收扩展到可见光区域，暴露出更多的催化活性位点，并抑制光诱导电荷的重组。因此，MV-Ce-MOFs 在可见光下具有很高的光催化 O2 演化活性，在 405 纳米的单色光照射下，表观量子效率（AQY）达到了令人印象深刻的 1.6%。MOF 金属节点价态的调节工程预示着设计基于 MOF 的光催化剂的新范例。

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来源期刊

Rare Metals 工程技术-材料科学：综合

CiteScore

12.10

自引率

12.50%

发文量

2919

审稿时长

2.7 months

期刊介绍： Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.