Silicon Carbide (SiC) and Silicon/Carbon (Si/C) Composites for High-Performance Rechargeable Metal-Ion Batteries

Abstract

Silicon carbide (SiC) and silicon nanoparticle-decorated carbon (Si/C) materials are electrodes that can potentially be used in various rechargeable batteries, owing to their inimitable merits, including non-flammability, stability, eco-friendly nature, low cost, outstanding theoretical capacity, and earth abundance. However, SiC has inferior electrical conductivity, volume expansion, a low Li⁺ diffusion rate during charge-discharge, and inevitable repeated formation of a solid-electrolyte interface layer, which hinders its commercial utilization. To address these issues, extensive research has focused on optimizing preparation methods, engineering morphology, doping, and creating composites with other additives (such as carbon materials, metal oxides, nitrides, chalcogenides, polymers, and alloys). Owing to the upsurge in this research arena, providing timely updates on the use of SiC and Si/C for batteries is of great importance. This review summarizes the controlled design of SiC-based and Si/C composites using various methods for rechargeable metal-ion batteries like lithium-ion (LIBs), sodium-ion (SIBs), zinc-air (ZnBs), and potassium-ion batteries (PIBs). The experimental and predicted theoretical performance of SiC composites that incorporate various carbon materials, nanocrystals, and non-metal dopants are summarized. In addition, a brief synopsis of the current challenges and prospects is provided to highlight potential research directions for SiC composites in batteries.

Keywords: Li-ion; Na-ion; SiC; Zn-ion; batteries; composite.

Figure 2

(a) The formation scheme and (b) TEM image of C@void/Si-g. (c) Cycling test of Si, Si-G, C@Si-G, and C@void/Si-G. Adapted with permission from Ref. [60] 2023, Elsevier. (d) The formation process, (e) TEM image, Si₃₀@C₄₀/G₃₀ composite. (f) Galvanostatic charge/discharge profiles for Si₃₀@C₄₀/G₃₀ composites after various cycles at 0.2 A/g. Adapted with permission from Ref. [61]. 2016, Elsevier. The schematic illustration of preparation (Si/C-CNFs-x) (g) and Galvanostatic charge/discharge profiles (h) for Si/C-CNFs-20 composites at 600 mAh/g. Adapted with permission from Ref. [73] 2015, Elsevier. (i) The SEM image and EDX mapping of SiC-Graphit-180 and (j) its cycling durability relative to Si/C-Graphite-x at 0.1 A/g. Adapted with permission from Ref. [76]. 2018, Springer.

Figure 4

(a) Illustration of the spray-drying process. Adapted with permission from Ref. [87] 2015, Elsevier. (b) Schematic of the preparation process of Si@C@RGO, its TEM image (c), and (d) its HRTEM image. (e) Cyclic profile of Si, Si@C, and Si@C@RGO composites at 100 mA/g in the 1st three cycles and then at 0.2 A/g. (f) Rate performance of Si@C and Si@C@RGO composites under various currents. Adapted with permission from Ref. [91] 2017, Elsevier. Schematic illustration of the synthesis of Si/CNTs (g) and its (h) TEM image and (i) HRTEM image. (j) The capacity of pouch cells with a commercial graphite anode and a LiCoO₂ (LCO) cathode compared with commercial Samsung LIBs. Adapted with permission from Ref. [96] 2021, Elsevier.

Figure 6

(a) Molecular structure of bulk SiC materials. (b) Calculated Li diffusion barriers (eV) on 3C (111), 3C ($\overline{111}$), 2H (0001), and 2H (000$\overline{1}$) surfaces with the schematic representation of corresponding diffusion paths. (c) Formation energies (eV) of VC and VSi. (d) Lithiation energies (eV) at the most favorable silicon vacancy and carbon vacancy sites for different polytypes of silicon carbide by GGA-PBE. Adapted with permission from Ref. [112] 2020, Phys. Chem. C. (e) The most stable adsorption configurations of various S-containing species adsorption on g-SiC₂. (f) A comparison of the anchoring effect of g-SiC₂ with different siligraphene. (g) The binding energies (Eb, eV), and charge transfer (Q, |e|) of various S-containing species on g-SiC₂. (h) The computed projected density of states (PDOSs) of S (of Li₂S₄ and Si of g-SiC₂) and Li (of Li₂S₄ and C of g-SiC₂). (i) Ratio for vdW interaction for the adsorption of S-containing species on various siligraphenes. Adapted with permission from Ref. [123] 2018, Appl. Surf. Sci.

Figure 10

(a) The preparation methods for SiC/CaCO₃ samples. (b) The morphological changes in the porous SiC/CaCO₃ samples (5SiC300 and 5SiC100) before and after 40 calcination–carbonation cycles. (c) Heat storage density in kJ/kg for pure CaCO₃, bulk, and porous SiC/CaCO₃ samples as a function of the number of cycles. Adapted with permission from Ref. [156] 2023, J. Alloys Compd. (d) Schematic and SEM images showing cycling performance of the SiCN/S and SiCN-BN/S composites. (e) Lithiation curves and delithiation curves of SiCN/S and all SiCN-BN/S samples. (f) Electrochemical parameters of the sulfurized SiCN samples. Adapted with permission from Ref. [158] 2024, J. Alloys Compd. (g) Schematic representation of the fabrication processes for Ag-PSi, Ag-PSi@C, and Ag-PSi@SiC@C, as well as the insertion and extraction of Li⁺ (enlarged diagram). (h) SEM image of (Ag-PSi@SiC@C. (i–k) HR-TEM images of Ag-PSi@SiC@C. (l–n) EDS element mapping images of Ag-PSi@SiC@C. (o) Comparison of the electrochemical performance of the Si-based anode. Adapted with permission from Ref. [159] 2024, J. Colloid Interface Sci.

Figure 1

(a) Illustration of the main focus and content of this review. (b) The number of articles versus citations based on Web of Science and Scopus data using the keywords “SiC anode batteries” and “SiC composite batteries”.

Figure 3

(a) The formation scheme of Si/PC-x and proposed structures of other shapes. (b) Cycling durability at 0.2 A/g of Si/PC-30 compared with Si/PC-x. (c) Cycling durability at 0.4 A/g after the rate test for Si/PC-30. Adapted with permission from Ref. [81]. 2021, Elsevier. (d) Schematic illustration of the formation, (e) TEM image, (f) HRTEM image, and (g) scanning TEM with EDX mapping of Si-Cu3Si-CNT/G-C. (h) Cycling stability of Si-Cu3Si-CNT/G-C at 0.2 A/g relative to graphite at 0.1 A/g, and bulk Si at 0.2 A/g. (i) Rate capabilities of graphite at 0.3 A/g and Si-Cu3Si-CNT/G-C at 1.2 A/g. Adapted with permission from Ref. [82]. 2020, Elsevier.

Figure 5

(a) Diagram for the rotational CVD carbon system for the preparation of Si@C-x. (b) Cycling durability of Si@C-x at 0.3 A/g, showing the 1st two cycles at 0.1 A/g and their delithiation capacities (c) at various currents. Adapted with permission from Ref. [104] 2014, American chemical society (ACS). SEM images of (d) SiNW/GM and (e,f) C/SiNW/GM. EDX elemental mapping of (g,h) SiNW/GM and (i,j) C/SiNW/GM (k) Cycling performance of GM, NW/GM, and C/SiNW/GM at a current density of 0.2 C over 50 cycles (l) Nyquist plots of GM, SiNW/GM, and C/SiNW/GM. Adapted with permission from Ref. [105] 2021, ACS.

Figure 7

(a–f) the structural arrangement of quasi-three-dimensional tetragonal SiC polymorphs. (g–l) Analyzes the stability of the quasi-three-dimensional tetragonal silicon carbon (SiC) polymorphs. (m) Migration energy barrier of q3-t(SiC)₁₂ and q3-t(SiC)₂₀ with other anode materials for Na-ion batteries. Adapted with permission from Ref. [127]. 2023, ACS Appl. Energy Mater.

Figure 8

(a) Schematic plot for the difference in the amount of waste with/without N-APPJ (recycling waste). (b) SEM image of refined waste powder. (c) Cycling test and coulombic efficiency of N000, N501, and N505. (d) Nyquist plots after the first charging process involving a fitted electronic circuit. Adapted with permission from Ref. [129] 2015, ACS Appl. Mater. Interfaces. (e) Schematic of the cell configuration and the corresponding electrode structure of NGSCW and NG after cycling. (f) SEM, TEM. (g) Impedance parameters derived using the equivalent circuit model. Adapted with permission from Ref. [130] 2017, J. Mater. Chem. A. SEM images comparing the surface morphology of Si, thin SiC, and thick SiC films, respectively, (h–j) before and (k–m) after cycling. (n) Cycling characteristics of Si, thin SiC, and thick SiC films at a 0.3 C charge/discharge current. Adapted with permission from Ref. [131] 2018, RSC Adv.

Figure 9

(a) Schematic plots of the mixed mechanisms of K+ storage and diffusion processes of K+ ions inside the SiC-CDC anodes. (b) TEM images of SiC-CDC-900 and SiC-CDC-1000 anodes. Adapted with permission from Ref. [145] 2020, Adv. Funct. Mater. (c) Schematic of the synthesis process and mechanism of SiC-doped NePCMs, (d) SEM and TEM images of SiC-doped NePCMs. (e) Phase-change properties of DHPD and NePCM with different ratios of SiC. Adapted with permission from Ref. [146] 2022, ACS Appl. Energy Mater. (f) Schematic illustration of the synthesis of bulk g-C₃N₄, silicon-oxy carbide, and N-graphene/SiOC. (g) SEM (h) TEM (i) EDX mapping of N-graphene/SiOC. (j) The BET surface area, pore volume, and average pore size of g-C₃N₄, SiOC, and N-graphene/SiOC. Adapted with permission from Ref. [147] 2023, J. Energy Storage.