Preparation and lithium storage properties of flexible self-standing PDDA-Si/G nanocomposite film

doi:10.11949/j.issn.0438-1157.20181287

Abstract

Abstract:

Silicon is an active electrode material for future commercial lithium-ion batteries with extremely high theoretical specific capacity (4200 (mA·h)/g). However, the large volume change of silicon over charge-discharge cycles weakens its competitiveness in the capacity and cycle life. A flexible self-supporting polydiene dimethylammonium chloride-Si/graphene (PDDA-Si/G) nanocomposite film was successfully prepared by electrostatic self-assembly technique. The composite film can maintain the integrity of electrode structure without adding binder and conductive carbon black. Graphene provides complete conductive network and mechanical toughness. The electrochemical test results show that when the current density was 0.2 A/g, the specific capacity of PDDA-Si/G composite could reach 1439.9 (mA·h)/g and the Coulombic efficiency was above 98%. The specific capacity was 1209.3 (mA·h)/g after 80 cycles. The specific capacity still maintained 499.9 (mA·h)/g at a high current density (2 A/g).

Key words: composites, nanostructure, silicon, graphene film, electrochemistry

摘要：

通过静电自组装技术成功制备得到柔性自支撑聚二烯二甲基氯化铵-Si/石墨烯(PDDA-Si/G)纳米复合薄膜。该复合薄膜无添加黏结剂及导电炭黑且仍能保持电极结构的完整性，其中石墨烯提供完整的导电网络和机械韧性。电化学测试结果表明，当电流密度为0.2 A/g，复合材料的比容量可达1439.9 (mA·h)/g，库仑效率保持98%以上。且在高电流密度(2 A/g)下，复合材料的比容量仍可维持在499.9 (mA·h)/g，远高于商品化纯Si电极的电化学性能。

关键词: 复合材料, 纳米结构, 硅, 石墨烯薄膜, 电化学

CLC Number:

TM 912.9

Yating ZHANG, Kaibo ZHANG, Kaili JIA, Xinfu HE, Guoyang LIU, Wei WANG, Yongling ZHANG, Jieshan QIU. Preparation and lithium storage properties of flexible self-standing PDDA-Si/G nanocomposite film[J]. CIESC Journal, 2019, 70(3): 1144-1151.

张亚婷, 张凯博, 贾凯丽, 贺新福, 刘国阳, 王伟, 张永玲, 邱介山. 柔性自支撑PDDA-Si/G纳米复合薄膜的制备及储锂性能[J]. 化工学报, 2019, 70(3): 1144-1151.

Figures/Tables 8

Fig.1 Schematic diagram of preparation of PDDA-Si/G composite film based on GO

Fig.2 Zeta potential of PDDA-Si/G and GO at different pH

Fig.3 SEM photograph of flexible self-standing PDDA-Si/G film(a),(b); cross-sectional SEM image of composite material(c) and mapping images of C, O and Si elements of PDDA-Si/G(d)

Fig.4 X-Ray diffraction patterns(a) and Raman spectra (b) for Si, GO, G and PDDA-Si/G film

Fig.5 TGA curves of Si, G and PDDA-Si/G film under air atmosphere

Fig.6 Cyclic voltammogram of PDDA-Si/G at 0.2 mV/s(a); constant current charge-discharge curves of composite at 0.2 A/g(b); cycle performance curves of PDDA-Si, Si, G and Coulombic efficiency(c); rate performance curve of composite film(d)

Fig.7 AC impedance spectroscopy of Si, PDDA-Si/G electrodes (a) and equivalent circuits diagram (b)

Table 1 Impedance parameters of Si and PDDA-Si/G electrodes for charge-discharge cycle

Sample	Cycle	R _s/Ω	R _SEI/Ω	R _ct/Ω
pure Si	0	4.16	—	297.63
PDDA-Si/G	0	3.12	—	165.68
PDDA-Si/G	80	3.02	11.3	58.68

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