High-Entropy Ultrathin Amorphous Metal–Organic Framework-Stabilized Ru(Mo) Dual-Atom Sites for Water Oxidation

IF 19.3 1区材料科学 Q1 CHEMISTRY, PHYSICAL ACS Energy Letters Pub Date : 2024-11-06 DOI:10.1021/acsenergylett.4c02552

Xueqin Mu, Min Yu, Xingyu Liu, Yuru Liao, Fanjiao Chen, Haozhe Pan, Ziyue Chen, Suli Liu, Dingsheng Wang, Shichun Mu

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Abstract

High-entropy metal–organic frameworks (HE-MOFs) offer immense potential in electrocatalysis due to their diverse metallic compositions and high densities of active sites. Integrating bimetallic single-atom catalysts (SACs) with HE-MOFs for enhanced oxygen evolution reaction (OER) performance remains challenging. Here, we stabilize atomically dispersed Ru and Mo in amorphous HE-MOF nanosheets (HE(Ru,Mo)-MOFs) via in situ-formed amorphous high-entropy oxides, elucidating the deprotonation mechanism. Evidence supports the presence of high-density O-bridged Ru and Mo dual-atom sites. The multimetallic composition induces electronic redistribution and balances the oxidation state of metal sites, enhancing intrinsic OER activity. HE(Ru,Mo)-MOFs exhibit low OER overpotentials of 267 mV@10 mA cm^–2 and 266 mV@10 mA cm^–2 in alkaline freshwater and industrial wastewater, respectively, with exceptional durability surpassing that of commercial RuO₂ catalysts. Mechanistic insights reveal that high atomic dispersion facilitates rapid charge transfer and intermediate transformation, promising advanced catalysts for energy conversion.

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用于水氧化的高熵超薄无定形金属有机框架-稳定 Ru(Mo) 双原子位点

高熵金属有机框架（HE-MOFs）因其多样化的金属成分和高密度的活性位点而在电催化方面具有巨大的潜力。将双金属单原子催化剂（SAC）与 HE-MOFs 相结合以提高氧进化反应（OER）的性能仍然具有挑战性。在这里，我们通过原位形成的无定形高熵氧化物，将原子分散的 Ru 和 Mo 稳定在无定形 HE-MOF 纳米片（HE(Ru,Mo)-MOFs）中，并阐明了去质子化机理。证据支持高密度 O 桥接 Ru 和 Mo 双原子位点的存在。多金属成分诱导了电子再分布，平衡了金属位点的氧化态，提高了固有的 OER 活性。在碱性淡水和工业废水中，HE(Ru,Mo)-MOFs 的 OER 过电位分别为 267 mV@10 mA cm-2 和 266 mV@10 mA cm-2，耐久性超过了商用 RuO2 催化剂。机理分析表明，高原子分散度有利于电荷快速转移和中间转化，有望成为能源转换的先进催化剂。

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来源期刊

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.