Macroporous Directed and Interconnected Carbon Architectures Endow Amorphous Silicon Nanodots as Low-Strain and Fast-Charging Anode for Lithium-Ion Batteries

doi:10.1007/s40820-023-01308-x

Abstract

Abstract:

Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries. Herein, we report a unique silicon-carbon composite fabricated by uniformly dispersing amorphous Si nanodots (SiNDs) in carbon nanospheres (SiNDs/C) that are welded on the wall of the macroporous carbon framework (MPCF) by vertical graphene (VG), labeled as MPCF@VG@SiNDs/C. The high dispersity and amorphous features of ultrasmall SiNDs (~ 0.7 nm), the flexible and directed electron/Li⁺ transport channels of VG, and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites, rapid Li⁺ transport path, and unique low-strain property during Li⁺ storage. Consequently, the MPCF@VG@SiNDs/C exhibits high cycle stability (1301.4 mAh g⁻¹ at 1 A g⁻¹ after 1000 cycles without apparent decay) and high rate capacity (910.3 mAh g⁻¹, 20 A g⁻¹) in half cells based on industrial electrode standards. The assembled pouch full cell delivers a high energy density (1694.0 Wh L⁻¹; 602.8 Wh kg⁻¹) and an excellent fast-charging capability (498.5 Wh kg⁻¹, charging for 16.8 min at 3 C). This study opens new possibilities for preparing advanced silicon-carbon composite anodes for practical applications.

Key words: Amorphous Si nanodots, Low-strain, Fast-charging, Lithium-ion batteries

Zhenwei Li, Meisheng Han, Peilun Yu, Junsheng Lin, Jie Yu. Macroporous Directed and Interconnected Carbon Architectures Endow Amorphous Silicon Nanodots as Low-Strain and Fast-Charging Anode for Lithium-Ion Batteries[J]. Nano-Micro Letters, 2024, 16(1): 98-.

Zhenwei Li, Meisheng Han, Peilun Yu, Junsheng Lin, Jie Yu. [J]. Nano-Micro Letters, 2024, 16(1): 98-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-023-01308-x

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/98

Figures/Tables 6

Fig. 1 Structural characterizations of samples. a Schematic of the synthesis process of samples. b SEM, c AC-TEM, d SAED, e HAADF, and f, g AC-TEM EDS mapping images of the SiNDs/C. h, i TEM and j HRTEM images of the VG@SiNDs/C. k SEM (inset is a high magnification of k), l TEM, and m HRTEM images of the MPCF@VG@SiNDs/C

Fig. 2 Sample analysis. a XRD patterns, b Raman spectra, and c XPS spectra of SiNDs/C, VG@SiNDs/C, and MPCF@VG@SiNDs/C. d Si 2p spectrum of SiNDs/C. e C 1s spectra, f TGA spectra, g nitrogen adsorption/desorption isotherms, h pore size distribution, and i tap/electrode density of SiNDs/C, VG@SiNDs/C, and MPCF@VG@SiNDs/C

Fig. 3 Lithium-ion storage performances. a First charge/discharge curves, b cycling performance at 0.1 A g⁻¹, c rate performance, d-f charge/discharge curves at different current densities, Nyquist plots g before cycling, h after the 1st cycle, and i after rate test of SiNDs/C, VG@SiNDs/C, and MPCF@VG@SiNDs/C

Fig. 4 Long-term cycle stability and kinetic analysis of MPCF@VG@SiNDs/C and performance comparison. a Charge-discharge profiles at the 1st, 2nd, and 100th cycles at 0.1 A g⁻¹, long-term cycling performances at b 1 A g⁻¹ and c 5 A g⁻¹, d CV profiles at different scan rates, e Log i_p against Log v at marked peaks, f the percentages of pseudocapacitive contribution at different sweep rates, g the detailed pseudocapacitive contribution at 1 mV s⁻¹. Performance comparison of the MPCF@VG@SiNDs/C with recently reported silicon-carbon anodes based on industrial electrode standards h and non-industrial electrode standards i for LIBs

Fig. 5 Low-strain property characterization. Top-view SEM images of the MPCF@VG@SiNDs/C electrodes a before cycling and b, c after 1000 cycles at 1 A g⁻¹. Side-view SEM images of the MPCF@VG@SiNDs/C electrodes d before cycling and e after 1000 cycles at 1 A g⁻¹. f High-magnification SEM images of the MPCF@VG@SiNDs/C after 1000 cycles at 1 A g⁻¹. g Stress distribution over A-SiNDs/C and C-SiNDs/C after volume expansion up to 400%. h Volumetric strain of A-SiNDs/C and C-SiNDs/C after volume expansion up to 400%. i Average stress and j strain variation of A-SiNDs/C and C-SiNDs/C during the expansion process. k Schematic diagram of the low-strain property

Fig. 6 Full cells testing and performance comparison. a Galvanostatic charge/discharge voltage curves at 0.1 C (inset is the prepared pouch full cell), cycling performance at b 0.1 C and c 1 C, d rate performance, and e relationship between energy density and charging time of the pouch full cell. f Cycle stability, g gravimetric, and h volumetric energy densities comparison with previously reported silicon-carbon anodes. i Photographs of the drone in flight powered by the prepared pouch full cell

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