Electrochemical properties of NiO–Ni nanocomposite as anode material for lithium ion batteries

doi:10.1016/j.jpowsour.2006.03.039

Journal of Power Sources

Volume 161, Issue 1, 20 October 2006, Pages 541-544

https://doi.org/10.1016/j.jpowsour.2006.03.039 Get rights and content

Abstract

NiO–Ni nanocomposite was prepared by calcining a mixture of Ni₂(OH)₂CO₃ and ethanol in a tube furnace at 700 °C for 45 min in air. The microstructure and morphology of the powders were characterized by means of X-ray diffraction (XRD) and transmission electron microscopy (TEM). In the composite, nanoscale Ni particles (<10 nm) were dispersed in the NiO matrix (about 100 nm). Electrochemical tests showed that the nanocomposite had higher initial and reversible capacity than pure NiO. The presence of the nanoscale Ni phase had improved both of the initial coulombic efficiency and the cycling performance, due to its catalytic activity, which would facilitate the decomposition of Li₂O and the SEI during the charge process.

Introduction

During the past decade, the research on anode materials for lithium ion batteries mainly focused on searching for carbon alternatives with larger capacities and better cycling performances [1]. These materials were: (i) alloys with an active component and inactive components toward Li which acted as buffering matrix, (ii) amorphous tin-based oxides (ATCO) proposed by Fuji Co [2], and (iii) layer structured materials such as Li_3−xCo_xN and Li_3−xNi_xN. Recently, Tarascon and co-workers reported that transition-metal oxides (MO, where M is Fe, Co, Ni, Cu or Mn which were inactive towards Li) could be a new class of anode materials for lithium ion batteries. These transition-metal oxides demonstrated electrochemical capacities of about 700 mAh g⁻¹ and excellent cycling performances [3]. These oxides with rock-salt structure have no sites for insertion/deinsertion of Li ions. There is a new mechanism which can be written as: M_xO_y + 2yLi ↔ yLi₂O + xM. During the discharge, the M_xO_y particle is completely disintegrated into highly dispersed metallic nanoparticles (<10 nm) and Li₂O matrix, but the global shape of the starting particle is preserved. During the subsequent charge, the Li₂O matrix decomposes and M nanoparticles convert back to M_xO_y nanograins. The occurring of this thermodynamically infeasible reaction is attributed to the highly active metallic nanoparticles [1]. Solid electrolyte interface (SEI) will also be formed during the discharge process, but it can be partially decomposed during the subsequent charge process, which is attributed to the catalytic activity of metallic nanoparticles [4]. The partially reversible formation/decomposition of SEI will lead to an extra capacity.

NiO has a theoretic capacity of 718 mAh g⁻¹ when it is used as anode material for lithium ion batteries. The cycling performance of NiO is worse than that of other transition metal oxides such as CoO, CuO, and Cu₂O, but it has a higher reversible capacity than CuO and Cu₂O [3], [5], and it is less expensive than CoO. Since the mechanism involves the reduction and oxidation of the active Ni nanoparticles, an increase in the content of the nanoscale Ni has the possibility to facilitate the decomposition of Li₂O and the SEI film during the charge process. In this present work, NiO–Ni nanocomposite was synthesized by a simple method, and the electrochemical properties of the nanocomposite as anode material for lithium-ion batteries were investigated.

Section snippets

Experimental

Ni₂(OH)₂CO₃ precursor was prepared as follows. Ni(NO₃)₂·6H₂O was dissolved in a ethanol–water (1:4 v/v) solvent and a green solution was formed. NH₄HCO₃ solution was added by drop under magnetic stirring until the pH value reached 7.5 upon which a light green precipitate formed. The precipitation was centrifugalized and washed with distilled water first, and then with ethanol, for three times respectively. Afterwards, the precipitation was calcined in air in a quartz tube furnace, which had been

Characterization of materials

The XRD patterns of the as-synthesized powders are given in Fig. 1. Pattern (a) shows Bragg reflections of NiO and Ni phase. This indicates that the sample prepared in air is composite of NiO and Ni. The weak Ni peaks indicate a low quantity of Ni. In pattern (b), all peaks can be index to a single NiO phase. This indicates that the sample prepared in oxygen is pure NiO.

EDS results show that the content of element Ni and O for the NiO sample are 47.84 and 52.16 at.%, respectively. The content of

Conclusions

NiO–Ni nanocomposite material was synthesized successfully. This material has higher initial and reversible discharge capacity, higher initial coulombic efficiency, and much better cycling performance than the pure NiO. And at the early stage of cycling, the reversible capacities of the NiO–Ni nanocomposite are higher than the theoretic value of NiO. The improvement of these properties can be attributed to the presence of nanoscale Ni particles in the composite, and quantities of defects

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