Rational construction of phosphate layer to optimize Cu-regulated Fe3O4 as anode material with promoted energy storage performance for rechargeable Ni-Fe batteries

doi:10.1016/j.jmst.2021.09.015

Abstract

Abstract:

Flexible aqueous energy storage devices with high security and flexibility are crucial for the progress of wearable energy storage. Particularly, aqueous rechargeable Ni-Fe batteries owning a large theoretical capacity, low cost and outstanding safety characteristics have emerged as a promising candidate for flexible aqueous energy storage devices. Herein, Cu-doped Fe₃O₄ (CFO) with 3D coral structure was prepared by doping Cu²⁺ based on Fe₃O₄ nanosheets (FO). Furthermore, the Fe-based anode material (CFPO) grown on carbon fibers was obtained by reconstructing the surface of CFO to form a low-crystallization shell which can enhance the ion transport. Excitingly, the newly developed CFPO electrode as an innovative anode material further exhibited a high capacity of 117.5 mAh g^-1 (or 423 F g^-1) at 1 A g^-1. Then, the assembled aqueous Ni-Fe batteries with a high cell-voltage output of 1.6 V deliver a high capacity of 49.02 mAh g^-1 at 1 A g^-1 and retention ratio of 96.8% for capacitance after 10 000 continuous cycles. What's more, the aqueous quasi-solid-state batteries present a remarkable maximal energy density of 45.6 Wh kg^-1 and a power density of 12 kW kg^-1. This work provides an innovative and feasible way and optimization idea for the design of high-performance Fe-based anodes, and may promote the development of a new generation of flexible aqueous Ni-Fe batteries.

Key words: Ni-Fe batteries, High voltage window regulation, High energy and power density, Anode materials, Amorphous phosphate layer

Shuhua Hao, Yupeng Xing, Peiyu Hou, Gang Zhao, Jinzhao Huang, Shipeng Qiu, Xijin Xu. Rational construction of phosphate layer to optimize Cu-regulated Fe₃O₄ as anode material with promoted energy storage performance for rechargeable Ni-Fe batteries[J]. J. Mater. Sci. Technol., 2022, 108: 133-141.

Figures/Tables 5

Fig. 1. Schematic illustration of the proposed samples grown on carbon fibers.

Fig. 2. SEM image of (a) FO nanosheet; The inset illustrates the complete and regular nanosheet structure; (b) CFO-0.5. The inset illustrates the accumulation of granular nanostructures; (c) CFO-1.5. The inset illustrates the excessive accumulation of granular nanostructures; (d-f) CFO-1. The inset illustrates a corresponding high-magnification SEM image with rough surface and coral; (g) CFPO and (h) Corresponding high-magnification SEM image with an amorphous layer. (h inset) The location of the element mapping image, the arrow point to the corresponding elements as follows: Cu, Fe, P, O.

Fig. 3. (a) XRD patterns of FO, CFO and CFPO samples grown on carbon fibers. XPS spectra of CFO and CFPO samples: (b) survey scan; (c-f) high-resolution spectra of the Cu 2p (c), Fe 2p (d), P 2p (e), O 1 s (f).

Fig. 4. (a) GCD curves of FO and CFO samples grown on carbon fibers at 1 A g-1. (b) Specific capacities of FO and CFO. (c) CV curves of the samples with different concentrations of copper at a scan rate of 20 mV s-1. (d) CV curves of CFO-1 at different scan rates from 20 to 100 mV s-1. (e) GCD curves of CFO-1. (f) CV curves of CFO-1 and CFPO. (g) CV curves of CFPO at different scan rates from 20 to 100 mV s-1. (h) GCD curves of CFPO. (i) Specific capacitances of the corresponding samples, at various current densities, as obtained from the GCD curves. (j) Cycling performance of the corresponding samples at 5 A g-1. (k) the EIS curves of the FO, CFO and CFPO electrodes.

Fig. 5. (a) CV curves of NiCo2S4 (positive electrode) and CFPO (negative electrode) at 5 mV s-1 based on three electrodes system; (b) CV curves of the as-assembled hybrid battery device at 100 mV s-1 ranging from 1.4-1.7 V; (c) CV curves of the as-assembled hybrid battery at various scan rate from 20-100 mV s-1; (d) specific capacitances of the hybrid battery. Inset: GCD curves of the device; (e) specific capacitances of hybrid battery at various current densities from 1 to 40 A g-1. Inset: discharge curves; (f) long-term cycling performance at 5 A g-1 for 10 000 cycles. Inset: physical picture of hydrogel for solid-state battery and electronic watches powered by two batteries; (g) ragone plot of the as-assembled solid-state battery; (h) schematic illustration of the hybrid battery based on NiCo2S4 (positive electrode) and CFPO (negative electrode).

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Rational construction of phosphate layer to optimize Cu-regulated Fe₃O₄ as anode material with promoted energy storage performance for rechargeable Ni-Fe batteries

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