Issue 12, 2024

Bulk-to-surface co-modification of layered hydrated vanadate cathode for aqueous zinc ion batteries

Abstract

The major challenges of vanadium-based layered materials are their dissolution tendency and the instability of their bulk-phase structure, resulting in unsatisfactory cyclability, particularly at lower current densities. Herein, we propose a co-modification strategy of dual-ion doping and forming an in situ cathode-electrolyte interphase (CEI). The dual ions, consisting of an alkali-metal ion (Na+ or K+) and an alkaline-earth-metal ion (Ca2+ or Ba2+), stabilize the bulk phase. The latter forms a precipitate with SO42− in the electrolyte as an in situ CEI with a balance of stability and pH adaptiveness. Based on the stabilized cathode from bulk phase to surface, Ca0.56Na1.19V6O16·4.09H2O exhibits excellent cyclability, especially at lower current densities. The full cell retains 99.4% of capacity after 120 cycles at 0.2 A g−1 and 25 °C while using Zn(OTF)2 electrolyte. Moreover, it exhibits 84.5% capacity retention at 0.1 A g−1 and −30 °C after 1000 cycles. The Zn2+/H+ intercalation mechanism was investigated by analytical characterizations and density functional theory (DFT) calculations, which implied that proton (de)intercalation is restrained at −30 °C, leading to the median discharge voltage increasing from 0.705 to 0.795 V. The co-modified cathode exhibits a significant performance in Zn(ClO4)2 electrolyte at 0.1 A g−1 and −30 °C (90.8% capacity retention after 2000 cycles). The co-modification strategy provides a viable option for cathode design.

Graphical abstract: Bulk-to-surface co-modification of layered hydrated vanadate cathode for aqueous zinc ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
02 Feb 2024
Accepted
03 May 2024
First published
06 May 2024

Energy Environ. Sci., 2024,17, 4090-4103

Bulk-to-surface co-modification of layered hydrated vanadate cathode for aqueous zinc ion batteries

C. Zhang, Y. Huang, X. Xu, Z. Chen, G. Xiao, Y. Zhong, X. Wang, C. Gu and J. Tu, Energy Environ. Sci., 2024, 17, 4090 DOI: 10.1039/D4EE00535J

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