Dual-Site Mn-Doped Vanadate Cathodes Involving Vanadium and Manganese Dual Redox Chemistry for High-Energy Aqueous Zinc-Ion Batteries

IF 18.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2025-09-19 DOI:10.1021/acsenergylett.5c02376

Xinghe Xu, , , Tianhao Wang, , , Xudong Zhao, , , Xuanhui Qu, , , Lifang Jiao, , and , Yongchang Liu*,

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Abstract

Popular vanadium-oxide and manganese-oxide based cathodes have garnered considerable attention for aqueous zinc-ion batteries (AZIBs) by virtue of their high discharge capacity and high working voltage, respectively. However, the low operating voltage of vanadium-oxide//Zn batteries and low specific capacity of manganese-oxide//Zn batteries significantly limit their practical applications. Herein, the V and Mn redox reactions are simultaneously activated in an intra-/interlayer dual-site Mn-doped Mn_0.4V_1.7O₅·0.5H₂O (MnVO) material to enhance the energy density. Specifically, the intralayer Mn-ions serve as redox centers to contribute capacity in the high-voltage region, while the interlayer Mn-ions mainly act as “pillars” to strengthen the layered structure. The combined spectroscopic/imaging analyses and theoretical computations elucidate the reversible V and Mn redox chemistry accompanied by H⁺/Zn²⁺ coinsertion/extraction in MnVO. Consequently, the tailored MnVO cathode achieves a significantly enhanced energy density (1.83 and 1.42 times those of vanadium-oxide and manganese-oxide, respectively) and an ultralong cycling durability (10000 cycles) in AZIBs.

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高能水锌离子电池中钒锰双氧化还原化学的双位置掺锰钒酸盐阴极

氧化钒基阴极和氧化锰基阴极分别以其高放电容量和高工作电压的优点在水锌离子电池中得到了广泛的应用。然而，氧化钒/锌电池的工作电压低，氧化锰/锌电池的比容量低，极大地限制了其实际应用。本文在层内/层间双位置Mn掺杂Mn0.4V1.7O5·0.5H2O （MnVO）材料中同时激活V和Mn的氧化还原反应，以提高能量密度。具体来说，层内的mn离子作为氧化还原中心在高压区贡献容量，而层间的mn离子主要作为“支柱”来加强层状结构。结合光谱/成像分析和理论计算，阐明了MnVO中伴随H+/Zn2+共插入/萃取的可逆V和Mn氧化还原化学反应。因此，定制的MnVO阴极在AZIBs中实现了显著提高的能量密度（分别是氧化钒和氧化锰的1.83倍和1.42倍）和超长循环耐久性（10000次循环）。

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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.