Weakly Polarized Organic Cation-Modified Hydrated Vanadium Oxides for High-Energy Efficiency Aqueous Zinc-Ion Batteries

doi:10.1007/s40820-024-01339-y

Abstract

Abstract:

Vanadium oxides, particularly hydrated forms like V₂O₅·nH₂O (VOH), stand out as promising cathode candidates for aqueous zinc ion batteries due to their adjustable layered structure, unique electronic characteristics, and high theoretical capacities. However, challenges such as vanadium dissolution, sluggish Zn²⁺ diffusion kinetics, and low operating voltage still hinder their direct application. In this study, we present a novel vanadium oxide ([C₆H₆N(CH₃)₃]_1.08V₈O₂₀·0.06H₂O, TMPA-VOH), developed by pre-inserting trimethylphenylammonium (TMPA⁺) cations into VOH. The incorporation of weakly polarized organic cations capitalizes on both ionic pre-intercalation and molecular pre-intercalation effects, resulting in a phase and morphology transition, an expansion of the interlayer distance, extrusion of weakly bonded interlayer water, and a substantial increase in V⁴⁺ content. These modifications synergistically reduce the electrostatic interactions between Zn²⁺ and the V-O lattice, enhancing structural stability and reaction kinetics during cycling. As a result, TMPA-VOH achieves an elevated open circuit voltage and operation voltage, exhibits a large specific capacity (451 mAh g^-1 at 0.1 A g^-1) coupled with high energy efficiency (89%), the significantly-reduced battery polarization, and outstanding rate capability and cycling stability. The concept introduced in this study holds great promise for the development of high-performance oxide-based energy storage materials.

Key words: Zinc-ion battery, Vanadium oxide, V₂O₅·nH₂O, Pre-intercalation, Interlayer engineering

Xiaoxiao Jia, Chaofeng Liu, Zhi Wang, Di Huang, Guozhong Cao. Weakly Polarized Organic Cation-Modified Hydrated Vanadium Oxides for High-Energy Efficiency Aqueous Zinc-Ion Batteries[J]. Nano-Micro Letters, 2024, 16(1): 129-.

Xiaoxiao Jia, Chaofeng Liu, Zhi Wang, Di Huang, Guozhong Cao. [J]. Nano-Micro Letters, 2024, 16(1): 129-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01339-y

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/129

Figures/Tables 7

Fig. 1 Structural and morphological characterization of TMPA-VOH and VOH. a XRD patterns. b TG curves. c SEM image, d, e TEM images and f the corresponding EDS elemental mappings of TMPA-VOH

Fig. 2 XPS analysis of TMPA-VOH and VOH. a XPS survey spectra, showing a clear N signal but no Cl signal in TMPA-VOH. High resolution of b C 1s spectra, a strong C-N peak in TMPA-VOH confirm the insertion of TMPA⁺ cations. c N 1s spectra, indicating the presence of C-N bonds and the formation of N-O bonds in TMPA-VOH. d V 2p and O 1s spectra, illustrating the introduction of a large amount of V⁴⁺ ions and the expulsion of interlayer water by TMPA⁺ pre-insertion. e VB spectra of TMPA-VOH and VOH

Fig. 3 Chemical interactions characterization by FTIR and EPR results. a FTIR spectra of TMPA-VOH and VOH. b FTIR spectra in the region of 1550-1200 cm⁻¹ show the characteristic vibration modes of TMPA⁺ species in TMPA-VOH. c FTIR spectra in the region of 1050-750 cm⁻¹ depict the splitting of the V = O peak and the absence of interlayer water in TMPA-VOH. d EPR spectra of TMPA-VOH and VOH show a stronger signal of unpaired electrons in TMPA-VOH, confirming the presence of more V⁴⁺ species

Fig. 4 The electrochemical performance of Zn//TMPA-VOH and Zn//VOH cells. a The 1st GCD curve at 0.1 A g^-1. b Rate performance and c the corresponding GCD profiles at various current densities. d Cycling performance at 4 A g^-1 and e GCD profiles of the 1st and 2000th cycle at 4 A g.^-1. f Energy efficiency at various current densities, providing an alternative perspective on rate capability. g Ragone plot (specific energy and specific power, based on the weight of the active material in cathode, are derived from the GCD data)

Fig. 5 a The 3rd cycle of CV tests at a scan rate of 0.1 mV s⁻¹. b The initial three cycles of CV tests at 0.1 mV s⁻¹ for TMPA-VOH. c CV curves at various scan rates for TMPA-VOH. d The log (peak current) vs. log (scan rate) plot for each redox peak in TMPA-VOH and their corresponding b values. e Contribution ratio and f specific capacitance of the diffusion-controlled process and capacitive process for TMPA-VOH and VOH at different scan rates

Fig. 6 Electrochemical reaction kinetics analysis. a Nyquist plots of TMPA-VOH and VOH electrodes before and after CV tests. b Plot of the real part of impedance vs. ω^−1/2 in the low-frequency region. c Zn ion diffusion coefficients and d internal resistance calculated from the 3rd cycle of GITT tests

Fig. 7 Energy storage mechanism of Zn//TMPA-VOH. a Ex situ XRD patterns. Ex situ XPS of b Zn 2p spectra, c V 2p spectra, and d O 1s spectra. e SEM elemental mapping images of TMPA-VOH cathode at discharged and charged state

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