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Si-Based Anodes: Advances and Challenges in Li-Ion Batteries for Enhanced Stability

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Abstract

Owing to their advantages, such as a high energy density, low operating potential, high abundance, and low cost, rechargeable silicon (Si) anode lithium-ion batteries (LIBs) have attracted considerable interest. Significant advancements in Si-based LIBs have been made over the past decade. Nevertheless, because the cycle instability is a crucial factor in the half/full-battery design and significantly affects the consumption of active components and the weight of the assembled battery, it has become a concern in recent years. This paper presents a thorough analysis of the recent developments in the enhancement methods for the stability of LIBs. Comprehensive in situ and operando characterizations are performed to thoroughly evaluate the electrochemical reactions, structural evolution, and degradation processes. Approaches for enhancing the cycle stability of Si anodes are systematically divided from a design perspective into several categories, such as the structural regulation, interfacial design, binder architecture, and electrolyte additives. The advantages and disadvantages of several methods are emphasized and thoroughly evaluated, offering insightful information for the logical design and advancement of cutting-edge solutions to address the deteriorating low-cycle stability of silicon-based LIBs. Finally, the conclusions and potential future research perspectives for promoting the cycling instability of silicon-based LIBs are presented.

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Fig. 1
Fig. 2

Reproduced with permission from Ref. [89]. Copyright © 2004, Elsevier. c The initial discharging/charging curve of pristine micro-Si anode materials. Reproduced with permission from Ref. [90]. Copyright © 2022, Elsevier

Fig. 3

Reproduced with permission from Ref. [110]. Copyright © 2022, Wiley-VCH

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Copyright © 2020, Elsevier

Fig. 7

Reproduced with permission from Ref. [37]. Copyright © 2020, Elsevier. Image of an Si-graphite anode taken by using XRD-CT: d an XRD-CT slice recorded at the start of the charge process displaying a phase-distribution pattern of crystalline Si (green), LixSi (blue), and LiC12 (red), where the teal is a blend of green (Si) and blue (lithiated Si) based on complementary color mixing; e magnified zones of focus revealing massive LixSi phase components in the graphite substrate with crystalline Si centers (1–3) and smaller LixSi particles (4). f Charge gradient and associated phases. g Over operating and open-circuit times, the d-spacing corresponds to the (002) reflection of the LixC6 architecture. h Magnified time span of Zone 1 demonstrating the incorporated peak regions of the LixC6 phases upon delithiation. i Magnified zone of concern displaying the c-lattice value of the solid-solution graphite phase over activation and open-circuit (green). Reproduced with permission from Ref. [117]. Copyright © 2019, American Chemical Society

Fig. 8

Reproduced with permission from Ref. [118]. Copyright © 2021, Elsevier

Fig. 9

Copyright © 2019, Royal Society of Chemistry. d, e In situ Raman spectra and mapping of Si@MoSe2 throughout the (de)lithiation procedure. Reproduced with permission from Ref. [120]. Copyright © 2022, American Chemical Society

Fig. 10

Reproduced with permission from Ref. [121]. Copyright © 2022, American Chemical Society

Fig. 11

Reproduced with permission from Ref. [124]. Copyright © 2021, Wiley-VCH. Architecture of g P-SiO and i D-SiO@G after 50 cycles and h, j corresponding chemical mapping, respectively. k Si K-edge XANES spectra of the four samples. l Morphology of cycled D-SiO@G particles and corresponding selected regions mapping, with modification. Reproduced with permission from Ref. [126]. Copyright © 2021, Wiley-VCH

Fig. 12

Reproduced with permission from Ref. [129]. Copyright © 2019, American Chemical Society. e HRTEM image of Si NW during (de)lithiation. f Enlarged HRTEM pattern of Si NW SEI. g EEL image of the C K-edge from the Si NW during (de)lithiation. h Si NW STEM EELS mapping at 1 V delithiation. Reproduced with permission from Ref. [130]. Copyright © 2019, Elsevier. HRTEM with the corresponding EDS images i, m after the initial discharge process and j, n initial charge process in FEC-free electrolyte, and k, o after initial lithiation and l, p initial delithiation in the FEC-containing electrolyte. Reproduced with permission from Ref. [131]. Copyright © 2021, Elsevier

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Fig. 14

Reproduced with permission from Ref. [136]. Copyright © 2021, Elsevier. e Scheme of hollow Si-C/graphite composites. f TEM and g, h HRTEM patterns of Si-C/G-A electrode materials. Reproduced with permission from Ref. [137]. Copyright © 2022, Elsevier. i Scheme of SiOx/C HS (GA, GL). SEM and TEM images of j–l SiOx/C HS-TA, (m–o) SiOx/C HS-GA, and p–r SiOx/C HS-GL with modifications. Reproduced with permission from Ref. [138]. Copyright © 2021. Wiley-VCH

Fig. 15

Reproduced with permission from Ref. [140]. Copyright © 2021, Elsevier. e Scheme of the design and synthesis of the hollow porous p-CoNC@SiX. SEM patterns of f ZnCo-ZIF, g ZnCo-ZIF@Si50, h ZnCo-ZIF@Si80, i ZnCo-ZIF@Si100 before pyrolysis, j p-CoNC, k p-CoNC@Si50, l p-CoNC@Si80, and m p-CoNC@Si100 after pyrolysis process. Reproduced with permission from Ref. [141]. Copyright © 2022, American Chemical Society. Preparation of n GP-Si and o NP-Si. Von Mises Stress distribution and volume change for GP-Si p before discharge, and at discharge times of q 10 h, r 20 h, and s 30 h (full discharge), with modifications. t Volume-specific capacity of two samples. Reproduced with permission from Ref. [142]. Copyright © 2021, Wiley-VCH

Fig. 16

Reproduced with permission from Ref. [149]. Copyright © 2022, American Chemical Society. g Scheme of synthesis process for H-SiNS/C material. h–j TEM, k, l HRTEM, and m cycling property of H-SiNS/C material. Reproduced with permission from Ref. [150]. Copyright © 2022, Wiley-VCH. n Synthesis procedure of LHGF/SiO materials. Scheme of the structural change in o pristine SiO anode and p LHGF/SiO anode. Reproduced with permission from Ref. [158]. Copyright © 2022, Springer Nature. q Galvanostatic charge/discharge plots of the two electrodes. r Rate behavior of LHGF/SiO-75% anode. s Scheme of SiO with two different metal hydrides (TiH2 and LiH). Reproduced with permission from Ref. [159]. Copyright © 2022, Elsevier

Fig. 17

Reproduced with permission from Ref. [63]. Copyright © 2021, Springer Nature. d Scheme of Li metal-free prelithiation induced phase change. e Results of the isosurface (atomic content of Si > 75%) investigation of SiO and prelithiated SiO materials. f Orthographic view of clipped volume, 2D contour plot of Si and O for the clipped volume, and clipped volume of prelithiated SiO (Li/Si = 0.67). Reproduced with permission from Ref. [62]. Copyright © 2021, Elsevier

Fig. 18

Reproduced with permission from Ref. [70]. Copyright © 2020, Elsevier. d Potential pathways for TTFPB’s electrochemical reductive breakdown. e Illustrative diagrams of defense process using implanted TTFPB nano-layer. f Estimated HOMO and LUMO energy for various molecules. g Cycling properties of pristine Si and Si@TTFPB at 0.2 C. Reproduced with permission from Ref. [166]. Copyright © 2022, Elsevier

Fig. 19
Fig. 20

Reproduced with permission from Ref. [191]. Copyright © 2022, Wiley-VCH. b Synthetic scheme of triblock polymer PSEA. c Scheme of π···π interaction between carbon and phenyl groups as well as hydrogen bonds between Si particles and carboxyl group of PSEA binder. Reproduced with permission from Ref. [194]. Copyright © 2022, Wiley-VCH. d Scheme of elastic properties of CPAU and e cycling performance of electrode materials. Reproduced with permission from Ref. [195]. Copyright © 2021, American Chemical Society. f Scheme of self-healing procedure and g cycling performance of electrode materials. Reproduced with permission from Ref. [196]. Copyright © 2022, Elsevier. h Comprehensive scheme of a gallol-conjugated binder’s molecular mobility in Si-microenvironments (Si-μ-env, the blue areas). Reproduced with permission from Ref. [197]. Copyright © 2021, Wiley-VCH

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Grant Nos. U22A20420, 22078029, 22208029, and 52203292), Postgraduate Research & Practice Innovation Program of Jiangsu Province (Grant No. KYCX23_3027) and the “333 high-level talent training project” young and middle-aged leading talent project of Jiangsu Province. The authors thank the Jiangsu Development and Reform Commission for their support.

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  1. School of Materials Science and Engineering, Jiangsu Province Engineering Research Center of Intelligent Manufacturing Technology for the New Energy Vehicle Power Battery, Changzhou Key Laboratory of Intelligent Manufacturing and Advanced Technology for Power Battery, Changzhou University, Changzhou, 213164, Jiangsu, China

    Hongshun Zhao, Jianbin Li, Qian Zhao, Shuyong Jia & Yurong Ren

  2. College of Chemistry and Materials Engineering, Hunan University of Arts and Science, Changde, 415000, Hunan, China

    Xiaobing Huang

  3. School of Chemistry, Tiangong University, Tianjin, 300387, China

    Jianmin Ma

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Zhao, H., Li, J., Zhao, Q. et al. Si-Based Anodes: Advances and Challenges in Li-Ion Batteries for Enhanced Stability. Electrochem. Energy Rev. 7, 11 (2024). https://doi.org/10.1007/s41918-024-00214-z

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