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Journal article
Operation of MXene-Derived Zinc-Preintercalated Bilayered Vanadium Oxide Cathode in Aqueous Zn-Ion Batteries
ACS applied energy materials, v 8(17), pp 12695-12711
08 Sep 2025
PMID: 40937098
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Abstract
Layered hydrated vanadium oxides, particularly those with bilayered structures, show remarkable electrochemical performance as cathodes for aqueous Zn-ion batteries (AZIBs). However, their wide-scale adoption is hindered by limited understanding of their charge storage mechanisms in different Zn-containing electrolytes. Here, we demonstrate the first synthesis of a MXene-derived Zn-preintercalated bilayered vanadium oxide (MD-ZVO) with a nanoflower-like morphology comprised of two-dimensional (2D) nanosheets, achieved via a two-step dissolution–recrystallization process. The strategic Zn2+ preintercalation establishes well-defined ion diffusion pathways, while the nanoflower-like assembly of 2D nanosheets enhances structural integrity, together contributing to improved electrochemical performance over other layered vanadium oxides. A systematic evaluation of four electrolytes (2 M ZnSO4, 2.6 M Zn(OTf)2, 2 M ZnCl2, and 30 m ZnCl2) showed that MD-ZVO electrodes delivered high reversible capacities (450 and 315 mAh g–1 at 0.1 A g–1), excellent rate capability (223 mAh g–1 for both electrolytes at 1.0 A g–1), and good electrochemical stability (84% and 48% over 1000 cycles at 1.0 A g–1) in saturated 2.6 M Zn(OTf)2 and highly concentrated 30 m ZnCl2, respectively. The material’s superior electrochemical stability in concentrated electrolytes is attributed to suppressed vanadium oxide dissolution during cycling. In situ and ex situ XRD analyses of MD-ZVO electrodes reveal larger contribution of Zn2+-associated species for charge storage in cells containing 2.6 M Zn(OTf)2 and proton dominant charge transfer in cells containing 30 m ZnCl2. Additionally, the combination of in situ and ex situ characterization demonstrates the reversible formation of ZnxOTfy(OH)2x–y·nH2O in cells using 2.6 M Zn(OTf)2 and Zn5(OH)8Cl2·H2O in cells using 30 m ZnCl2 on the MD-ZVO electrode surface over extended cycling. This work highlights the superior performance of nanoflower MD-ZVO for cathodes in aqueous Zn-ion batteries, which benefits from the proper selection of highly concentrated electrolytes that enable better utilization of the cathode material.
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Details
- Title
- Operation of MXene-Derived Zinc-Preintercalated Bilayered Vanadium Oxide Cathode in Aqueous Zn-Ion Batteries
- Creators
- Timofey K Averianov - Drexel University, Materials Science and EngineeringKyle Joseph Matthews - Drexel University, Materials Science and EngineeringXinle Zhang - Drexel University, Materials Science and EngineeringHuyen T. K. Nguyen - Drexel UniversityYuan Zhang - Drexel University, A.J. Drexel Nanomaterials InstituteYury Gogotsi - Drexel University, Materials Science and EngineeringEkaterina A Pomerantseva (Corresponding Author) - Drexel University, Materials Science and Engineering
- Publication Details
- ACS applied energy materials, v 8(17), pp 12695-12711
- Publisher
- ACS Publications
- Number of pages
- 17
- Grants
- Grant note
- Division of Materials Research: DMR-1752623, DMR-2427077 National Science FoundationMESC+ Erasmus Mundus program by the European UnionAlexander von Humboldt fellowship
This work was supported by the National Science Foundation grants DMR-1752623 and DMR-2427077. H.T.K.N. was supported through MESC+ Erasmus Mundus program by the European Union. Y.Z. was supported through the Alexander von Humboldt fellowship. We thank Dr. Christopher E. Shuck (Rutgers University, previously A.J. Drexel Nanomaterials Institute at Drexel University) for providing MAX phase materials and for scientific discussions. We thank Prof. Kevin Owens (Department of Chemistry, Drexel University) for providing access to atomic absorption spectroscopy characterization in the Instrumental Analytical Laboratory. We thank the Drexel Materials Characterization Core for providing access to SEM, EDS, XRD, and XPS instruments.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering; College of Engineering; A.J. Drexel Nanomaterials Institute
- Web of Science ID
- WOS:001559037700001
- Scopus ID
- 2-s2.0-105024553160
- Other Identifier
- 991022083454304721
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- Web of Science research areas
- Chemistry, Physical
- Energy & Fuels
- Materials Science, Multidisciplinary