Abstract
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.
| Original language | English (US) |
|---|---|
| Article number | 2403371 |
| Journal | Advanced Materials |
| Volume | 36 |
| Issue number | 30 |
| DOIs | |
| State | Published - Jul 25 2024 |
Funding
This work was supported by the National Natural Science Foundation of China (Grant Nos. 52172231, 52127816, and 52202290), the National Key Research and Development Program of China (Grant No. 2020YFA0715000), the Engineering and Physical Sciences Research Council (EPSRC, EP/V027433/3), UK Research and Innovation (UKRI) under the UK government's Horizon Europe funding (101077226; EP/Y008707/1), the Natural Science Foundation of Hubei Province (Grant No. 2022CFA087, and 2022CFD090), The Sanya Science and Education Innovation Park of Wuhan University of Technology (Grant No. 2022KF0011). This work gratefully acknowledges support from the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. This research used resources of the Advanced Photo Source (beamline 12‐BM), a U.S. DOE Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐ 06CH11357. Junjun Wang thanks the funding support from China Scholarship Council/University College London for the joint Ph.D. scholarship (Grant No. CXXM2110070005). The project supported by State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology).
Keywords
- Ca-ion batteries
- in situ characterizations
- lattice self-regulation
- layered vanadium oxides
- multivalent-ion batteries
ASJC Scopus subject areas
- General Materials Science
- Mechanics of Materials
- Mechanical Engineering