Freestanding Ammonium Vanadate Composite Cathodes with Lattice Self-Regulation and Ion Exchange for Long-Lasting Ca-Ion Batteries

Wang, Junjun; Zhang, Yadi; Qiao, Fan; Jiang, Yalong; Yu, Ruohan; Li, Jiantao; Lee, Sungsik; Dai, Yuhang; Guo, Fei; Jiang, Peie; Zhang, Lei; An, Qinyou; He, Guanjie; Mai, Liqiang

doi:10.1002/adma.202403371

Title: Freestanding Ammonium Vanadate Composite Cathodes with Lattice Self-Regulation and Ion Exchange for Long-Lasting Ca-Ion Batteries

Journal Article · 03 May 2024 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202403371 · OSTI ID:2506746

Wang, Junjun ^[1]; Zhang, Yadi ^[2]; Qiao, Fan ^[3]; Jiang, Yalong ^[4]; Yu, Ruohan ^[3]; Li, Jiantao ^[5]; Lee, Sungsik ^[5]; Dai, Yuhang ^[3]; Guo, Fei ^[6]; Jiang, Peie ^[6]; Zhang, Lei ^[3]; An, Qinyou ^[3];

^[6]; Mai, Liqiang ^[3]

Wuhan Univ. of Technology (China); Univ. College London (United Kingdom)
Shanghai Jiao Tong Univ. (China)
Wuhan Univ. of Technology (China)
Wuhan Textile University (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. College London (United Kingdom)

Calcium-ion batteries (CIBs) have emerged as a promising alternative for electrochemical energy storage. The lack of high-performance cathode materials severely limits the development of CIBs. Vanadium oxides are particularly attractive as cathode materials for CIBs, and preinsertion chemistry is often used to improve their calcium storage performance. However, the room temperature cycling lifespan of vanadium oxides in organic electrolytes still falls short of 1000 cycles. Here, based on preinsertion chemistry, the cycling life of vanadium oxides is further improved by integrated electrode and electrolyte engineering. Utilizing a tailored Ca electrolyte, the constructed freestanding (NH₄)₂V₆O₁₆·1.35H₂O@graphene oxide@carbon nanotube (NHVO-H@GO@CNT) composite cathode achieves a 305 mAh g^-1 high capacity and 10 000 cycles record-long life. Additionally, for the first time, a Ca-ion hybrid capacitor full cell is assembled and delivers a capacity of 62.8 mAh g^-1. The calcium storage mechanism of NHVO-H@GO@CNT based on a two-phase reaction and the exchange of NH₄⁺ and Ca²⁺ during cycling are revealed. The lattice self-regulation of V—O layers is observed and the layered vanadium oxides with Ca²⁺ pillars formed by ion exchange exhibit higher capacity. This work provides novel strategies to enhance the calcium storage performance of vanadium oxides via integrated structural design of electrodes and electrolyte modification.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; National Natural Science Foundation of Hubei Province

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2506746

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 30 Vol. 36; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Ca-ion batteries
in-situ characterizations
lattice self-regulation

Title: Freestanding Ammonium Vanadate Composite Cathodes with Lattice Self-Regulation and Ion Exchange for Long-Lasting Ca-Ion Batteries

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