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Nano-Micro Letters  2024, Vol. 16 Issue (1): 179-    DOI: 10.1007/s40820-024-01388-3
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Mustafa Khan1, Suxia Yan1(), Mujahid Ali2, Faisal Mahmood2, Yang Zheng1, Guochun Li1, Junfeng Liu1(), Xiaohui Song3, Yong Wang1()
Innovative Solutions for High-Performance Silicon Anodes in Lithium-Ion Batteries: Overcoming Challenges and Real-World Applications
Mustafa Khan1, Suxia Yan1(), Mujahid Ali2, Faisal Mahmood2, Yang Zheng1, Guochun Li1, Junfeng Liu1(), Xiaohui Song3, Yong Wang1()
1 Institute for Energy Research, Jiangsu University, Zhenjiang, 212013, Jiangsu, People’s Republic of China
2 School of Energy and Power Engineering, Jiangsu University, Zhenjiang, 212013, Jiangsu, People’s Republic of China
3 School of Materials Science and Engineering, Hefei University of Technology, Hefei, 230009, Anhui, People’s Republic of China
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Mustafa Khan
Suxia Yan
Mujahid Ali
Faisal Mahmood
Yang Zheng
Guochun Li
Junfeng Liu
Xiaohui Song
Yong Wang
Abstract：

Silicon (Si) has emerged as a potent anode material for lithium-ion batteries (LIBs), but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation, leading to material pulverization and capacity degradation. Recent research on nanostructured Si aims to mitigate volume expansion and enhance electrochemical performance, yet still grapples with issues like pulverization, unstable solid electrolyte interface (SEI) growth, and interparticle resistance. This review delves into innovative strategies for optimizing Si anodes’ electrochemical performance via structural engineering, focusing on the synthesis of Si/C composites, engineering multidimensional nanostructures, and applying non-carbonaceous coatings. Forming a stable SEI is vital to prevent electrolyte decomposition and enhance Li+ transport, thereby stabilizing the Si anode interface and boosting cycling Coulombic efficiency. We also examine groundbreaking advancements such as self-healing polymers and advanced prelithiation methods to improve initial Coulombic efficiency and combat capacity loss. Our review uniquely provides a detailed examination of these strategies in real-world applications, moving beyond theoretical discussions. It offers a critical analysis of these approaches in terms of performance enhancement, scalability, and commercial feasibility. In conclusion, this review presents a comprehensive view and a forward-looking perspective on designing robust, high-performance Si-based anodes the next generation of LIBs.
Key words： Silicon anode    Energy storage    Nanostructure    Prelithiation    Binder
收稿日期: 2023-12-30      出版日期: 2024-04-24
通讯作者: Suxia Yan, Junfeng Liu, Yong Wang   
引用本文:   
Mustafa Khan, Suxia Yan, Mujahid Ali, Faisal Mahmood, Yang Zheng, Guochun Li, Junfeng Liu, Xiaohui Song, Yong Wang. [J]. Nano-Micro Letters, 2024, 16(1): 179-.
Mustafa Khan, Suxia Yan, Mujahid Ali, Faisal Mahmood, Yang Zheng, Guochun Li, Junfeng Liu, Xiaohui Song, Yong Wang. Innovative Solutions for High-Performance Silicon Anodes in Lithium-Ion Batteries: Overcoming Challenges and Real-World Applications. Nano-Micro Letters, 2024, 16(1): 179-.
链接本文:  
https://www.qk.sjtu.edu.cn/nml/CN/10.1007/s40820-024-01388-3      或      https://www.qk.sjtu.edu.cn/nml/CN/Y2024/V16/I1/179
Fig. 1  
Anode material Theoretical gravimetric capacity (mAh g−1) Working potential (V) Volume variation (%)
Si 4200 0.4 400
Li 3862 0 100
Ge 1625 0.5 370
Sn 994 0.6 26
Graphite 372 0.05 12
Li4Ti5O12 175 1.5 1
TiO2 167 0.8  < 4
Table 1  
Phase Theoretical capacity (mAh g−1) Volume variation (%)
Si 0 0
LiSi 954 160
Li12Si7 1635 222
Li2Si 1900 263
Li13Si4 3100 389
Li15Si4 3590 390
Li22Si5 4200 400
Table 2  
Fig. 2  
Fig. 3  
Fig. 4  
Fig. 5  
Fig. 6  
Si Anodes Current density (A g−1) Cycle number Remaining capacity (mAh g−1) Refs.
Si/C 0.3 100 611.3 [62]
Si/p-C(N-SPC) 0.4 100 1607 [63]
Si@viod@C - 40 500 [64]
Si@C@viod@C 0.1 50  ~ 1350 [65]
Porous Si/C 0.5 30 759 [66]
Meso-Si/C 1 1000 990 [67]
Porous Si/C nanotubes 0.2 200 1300 [68]
Si/graphite/C 0.5 300  ~ 400 [69]
Si@C@CNTs&CNFs 0.3 50 1195 [70]
Si/CNTs 0.42 100 1000 [39]
Si/CNTs 42 100 800 [71]
Si@HC/CNFs 0.2 100  ~ 1020 [72]
Si/graphene 0.1 200 1500 [33]
Si/rGO 0.1 100 1433 [73]
Si/C/graphene 0.2 100 760 [74]
Si@C-rGO 0.3 400 931 [75]
M-pSi@C 1 250 1702 [76]
Si/C 0.1 100 941 [77]
Si/C 0.5 100 605.43 [78]
Si/C 2 400 1283 [79]
Si/C/rGO 1 270 1004 [80]
C-Si@graphite 4.2 1000  ~ 900 [81]
C@void/Si-G 8.4 200 1082.7 [82]
Si/Cu/Cu3Si@C 2.1 500 984 [83]
Table 3  
Fig. 7  
Fig. 8  
Fig. 9  
Si Anodes Current density (A g−1) Cycle number Remaining capacity (mAh g−1) Refs.
Si/meso-C 2 50 700 [111]
Si/void/C 0.1 80 980 [112]
Si/C 0.372 100 1500 [113]
Si/MWCNT 0.4 70 520 [114]
Si/CNTs 0.42 200 925 [115]
Si/graphene/graphite foam 0.4 100 370 [116]
Graphene/Si/C 0.3 100 902 [117]
Si NWs 0.26 100 2000 [118]
SiNTs 0.4 90  ~ 800 [119]
C@SiNTs 0.84 200 2085 [120]
CNTs/SiNTs 1.7 250 800 [121]
C@Si@CNTs 0.294 60 2200 [122]
Si@C/rGO 2 600 1100 [123]
Si/C 0.5 300 1041 [15]
Si/rGO 4 100 1521 [124]
SI/C 0.188 120 1179 [125]
Si/C-CNTs 0.5 200 1585.9 [126]
Si/C 4.2 500 1145 [127]
Si/NSs@C 0.1 200 822 [128]
C/Si 4 500 1072.2 [129]
Table 4  
Fig. 10  
Fig. 11  
Si Anodes Current density (A g−1) Cycle number Remaining capacity (mAh g−1) Refs.
Si/Ag 0.84 100 1163 [109]
Si/Cu 2.1 60 2002 [143]
Si/ZnO 0.84 210 1500 [144]
SiNPs/V2O5 2.1 50 932 [145]
SiNPs/LIPON 2.1 100 1050 [146]
SiNPs/GR/Li7P3S11 4.2 500 1332 [147]
SiNPs/GR/Li4SiO4 0.21 40 1893 [148]
P0.5% Si-Cu 0.1 60 1048 [149]
Si@LPO@void@FC 1 500 569 [150]
β-Si3N4/Si 5 100 480 [151]
Table 5  
Fig. 12  
Fig. 13  
Fig. 14  
Fig. 15  
Composite type Strategy/composition Description Scalability potential Commercial feasibility
1D Carbon-Si Composites CNFs and CNTs Integration with Si Utilization of CNFs and CNTs to construct conductive networks and host matrices for Si-based anode materials, handling volume changes during charging/discharging. Examples include C-L-SC, Si@CNTs, and Si/CNFs High scalability due to established manufacturing techniques for CNFs/CNTs Good, considering growing demand in energy storage technologies
2D Carbon-Si Composites Graphene and MXene Integration with Si Incorporation of graphene and MXenes with Si, resulting in structures like Si@G, Si@N-G, and MXene/Si@SiOx@C. Enhanced by the surface area and conductivity of graphene and the unique properties of MXenes Moderate, challenges in large-scale production of quality graphene and MXenes Promising, but dependent on cost reduction and production advancements
3D Carbon-Si Composites Porous Carbon and Graphite Integration with Si Development of composites like gigaporous carbon microspheres and Si/graphite/carbon (Si-G/C) composites, leveraging the structural benefits of 3D carbon materials High, given the existing large-scale production for porous carbon and graphite Very feasible, especially in markets demanding high-performance batteries
Table 6  
Nanostructure type Strategy/composition Description Scalability potential Commercial feasibility
0D Si-based anode materials Si nanoparticles and composites Utilization of porous Si nanoparticles and composites, including Si@TiO2 and Si/Ti2O3/rGO. Techniques include electroless etching, self-assembly, CVD Moderate, challenges in consistent quality production at scale Emerging, hinges on integration with current battery manufacturing processes
1D Si-based anode materials Si nanowires (SiNWs) and nanotubes (SiNTs) Development of 1D structures like SiNWs and SiNTs using CVD and other methods. Examples include Si@NC, carbon-coated SiNWs High for SiNWs with established methods; moderate for SiNTs due to complexity Promising, particularly for high-end applications requiring advanced battery properties
2D Si-based anode materials Si thin films Application of Si thin films on substrates, e.g., amorphous Si on Cu. Techniques include electrodeposition and magnetron sputtering Moderate, dependent on deposition technologies and material handling Feasible, with potential in niche markets and specialty applications
3D Si-based anode materials 3D macroporous Si structures Creation of 3D macroporous Si using methods like magnesiothermic reduction and galvanic displacement. Examples include Si@C electrodes and hollow Si nanospheres High, especially with advancements in 3D material synthesis techniques Good, subject to demonstration of long-term durability and cost-effectiveness
Table 7  
Material type Strategy/composition Description Scalability potential Commercial feasibility
SiOx/C composites Encapsulation of SiOx in Carbon Utilization of carbon matrices to encapsulate SiOx, enhancing electron/ion transport and forming a stable SEI layer. Examples include 3D-Si@SiOx/C, SiOx/C from rice husk High, leveraging existing carbon material production infrastructures Very promising, especially if cost-effectiveness is achieved
Si with non-carbonaceous materials Core-shell structures with metals/metal oxides Development of core-shell structures combining Si with metals/metal oxides like TiO2, SnO2, Nb2O5. Techniques include CVD, solvothermal methods Moderate, challenges in uniform core-shell structuring at scale Emerging, with potential in high-performance battery sectors
Table 8  
Aspect Strategy/Technique Description Scalability potential Commercial feasibility
Artificial solid electrolyte interphase (ASEI) for Si anode Engineered design of ASEI Construction of artificial SEI layers using ex situ and in situ techniques to provide a robust protective layer on the anode Moderate, requires precise control over layer formation Promising, essential for high-capacity, long-life batteries
Prelithiation of anode material Various prelithiation Techniques Techniques like lithium foil contact (LFC), stabilized Lithium Metal Powder (SLMP), and chemical prelithiation to compensate for lithium loss High, especially with advancements in lithiation technologies Very feasible, can significantly enhance the market competitiveness of Si-based LIBs
Effect of binder Use of advanced binders Exploration of alternative binders (e.g., alginate, PAA, SHP) tailored for Si-based anodes to accommodate extensive volume changes High, as alternative binders can be integrated into existing battery production lines Very promising, especially for advanced batteries requiring high stability and performance
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