Exploration of cobalt selenite-carbon composite porous nanofibers as anode for sodium-ion batteries and unveiling their conversion reaction mechanism

doi:10.1016/j.jmst.2021.01.076

Abstract

Abstract:

Efforts have been made to develop a promising anode material with a novel composition for sodium-ion batteries (SIBs). In this study, the sodium-ion storage mechanism of transition metal selenite that comprises transition metal cation coupled with two anions is studied. Amorphous cobalt selenite (CoSeO₃)-carbon composite nanofibers containing numerous pores are synthesized via electrospinning process. Upon heat treatment of the electrospun nanofibers containing selenium, CoSe₂ nanoclusters are formed. During the subsequent oxidation, CoSe₂ transformed into amorphous CoSeO₃ and some part of carbon was oxidized into CO₂, leaving the pores inside the nanofiber. To unveil the electrochemical reaction mechanism, analytical methods including cyclic voltammetry, ex-situ X-ray photoelectron spectroscopy, ex-situ transmission electron microscopy, and in-situ electrochemical impedance spectroscopy techniques were adopted. Based on the analyses, the following conversion reaction from the second cycle onward is suggested: CoO + xSeO₂ + (1 - x)Se + 4(x + 1)Na⁺ + 4(x + 1)e^- ↔ Co + (2x + 1)Na₂O + Na₂Se. Furthermore, the electrochemical properties of porous CoSeO₃-carbon composite nanofibers are analyzed in detail. The anode material exhibited stable cycle stability up to 200 cycles at 0.5 A g ^-1 and high rate performance up to 5 A g^-1.

Key words: Anode materials, Sodium-ion batteries, Conversion eaction, Metal selenite, Electrospinning

Jin-Sung Park, Gi Dae Park, Yun Chan Kang. Exploration of cobalt selenite-carbon composite porous nanofibers as anode for sodium-ion batteries and unveiling their conversion reaction mechanism[J]. J. Mater. Sci. Technol., 2021, 89: 24-35.

Figures/Tables 11

Scheme 1. Schematic illustration showing the formation mechanism of p-CoSeO3-CNF.

Fig. 1. Morphologies, SAED pattern, and elemental mapping images of CoSe2-CNF nanofibers: (a) SEM image, (b, c) TEM images, (d) HR-TEM image, (e) SAED pattern, and (f) elemental dot mapping images.

Fig. 2. Morphologies, SAED pattern, and elemental mapping images of p-CoSeO3-CNF: (a) SEM image, (b, c) TEM images, (d) HR-TEM image, (e) SAED pattern, and (f) elemental dot mapping images.

Fig. 3. XPS spectra of p-CoSeO3-CNF: (a) Co 2p, (b) Se 3d, (c) O 1s, and (d) C 1s.

Fig. 4. XPS spectra of p-CoSeO3-CNF electrode after the 1st (a-d) discharge and (e-h) charge processes: (a, e) Co 2p, (b, f) Na 2s & Se 3d, (c, g) Na 1s, and (d, h) O 1s.

Fig. 5. Ex-situ TEM images and corresponding SAED patterns of p-CoSeO3-CNF after the 1 st (a-c) discharge and (d-f) charge processes: (a, d) TEM images, (b, e) HR-TEM images, and (c, f) SAED patterns.

Fig. 6. (a) CV curves and (b) galvanostatic charge-discharge curve (for the initial cycle) of p-CoSeO3-CNF.

Fig. 7. (a) Potential vs. capacity graph where red dots correspond to the pre-selected potentials for which the Nyquist plots were obtained, (b) in-situ Nyquist plots, (c) Rct and (d) RSEI values obtained at preselected potential for the first cycle.

Scheme 2. Schematic illustration of the electrochemical reactions of CoSeO3 material during the first discharge process and subsequent cycles.

Fig. 8. Electrochemical properties of p-CoSeO3-CNF: (a) cycle performance at 0.5 A g-1 (where colored dots represent the cycle number for which the ex-situ Nyquist plots were obtained), (b) rate performance, (c-f) ex-situ Nyquist plots obtained for (c) the assembled cell and after the (d) 1 st, (e) 50th, and (f) 100th cycles.

Fig. 9. (a) CV graphs of p-CoSeO3-CNF obtained at various sweep rates, (b) linear fitting of log (peak current) vs. log (scan rate) data for Peak 1 (anodic) and Peak 2 (cathodic), (c) diagram showing the capacitive contribution (red-colored area) and the experimentally obtained current (in gray), and (d) percentages of capacitive contribution at numerous sweep rates.

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