Electrochemical performance of thermally-grown SiO<sub>2</sub> as diffusion barrier layer for integrated lithium-ion batteries

doi:10.1007/s11708-018-0556-0

Front. Energy

2018, Vol. 12

Issue (2) : 225-232 https://doi.org/10.1007/s11708-018-0556-0

RESEARCH ARTICLE

Electrochemical performance of thermally-grown SiO₂ as diffusion barrier layer for integrated lithium-ion batteries

X. D. HUANG¹(

), X. F. GAN¹, Q. A. HUANG¹(

), J. Z. YANG²

¹. Key Laboratory of MEMS of the Ministry of Education, School of Electronic Science and Engineering, Southeast University, Nanjing 210096, China
². School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

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Abstract

Direct integration of lithium-ion battery (LIB) with electronic devices on the same Si substrate can significantly miniaturize autonomous micro systems. For achieving direct integration, a barrier layer is essential to be inserted between LIB and the substrate for blocking Li⁺ diffusion. In this paper, the feasibility of thermal SiO₂ film as the barrier layer is investigated by electrochemical characterization and X-ray photoelectron spectroscopy (XPS). Due to the negligible side reactions of thermal SiO₂ with electrolyte, the solid electrolyte interphase (SEI) layer formed on the surface of the barrier layer is thin and the SEI content mainly consists of hydrocarbon together with slight polyethylene oxide (PEO), Li_xPO_yF_z, and Li₂CO₃. Although 8-nm thermal SiO₂ effectively prevents the substrate from alloying with Li⁺, the whole film changes to Li silicate after electrochemical cycling due to the irreversible chemical reactions of SiO₂with electrolyte. This degrades the performance of the barrier layer against the electrolyte penetration, thus leading to the existence of Li⁺ (in the form of F-Si-Li) and solvent decompositions (with the products of hydrocarbon and PEO) near the barrier layer/substrate interface. Moreover, it is found that the reaction kinetics of thermal SiO₂ with electrolyte decrease significantly with increasing the SiO₂ thickness and no reactions are found in the bulk of the 30-nm SiO₂ film. Therefore, thermal SiO₂with an appropriate thickness is a promising barrier layer for direct integration.

Keywords autonomous micro system direct integration barrier layer thermal SiO₂ film X-ray photoelectron spectroscopy (XPS)

Corresponding Author(s): X. D. HUANG,Q. A. HUANG

Just Accepted Date: 19 March 2018 Online First Date: 16 April 2018 Issue Date: 04 June 2018

Cite this article:

X. D. HUANG,X. F. GAN,Q. A. HUANG, et al. Electrochemical performance of thermally-grown SiO₂ as diffusion barrier layer for integrated lithium-ion batteries[J]. Front. Energy, 2018, 12(2): 225-232.

URL:

https://academic.hep.com.cn/fie/EN/10.1007/s11708-018-0556-0
https://academic.hep.com.cn/fie/EN/Y2018/V12/I2/225

Fig.1 Electrochemical characteristics of the samples

Fig.2 XPS Si 2p spectrum for the sample with 8-nm SiO₂ before and after galvanostatic cycling

Fig.3 Spectra on the barrier layer surface (no sputtering) and after 0.6-min sputtering for the sample with 8-nm SiO₂ after cycling

Fig.4 XPS depth profiling for the sample with 8-nm SiO₂ after cycling (The P 2p content decreases to a negligible level upon sputtering and thus is not shown.)

Fig.5 Spectra near the barrier layer/substrate interface for the sample with 8-nm SiO₂ after cycling (The inset of Fig. 5(a) is the amplified Si 2p spectrum after 3.6-min sputtering, where a weak peak corresponding to the barrier layer is observed.)

Fig.6 Spectra on the barrier layer surface (no sputtering) and after 3.6-min sputtering for the sample with 30-nm SiO₂ after cycling (Note that Figs. 6(a) and 6(b) have the same x- and y-coordinates as Figs. 3(b) and 3(c) respectively for fair comparison.)

Fig.7 Surface morphologies of the samples

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