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摘要: 金属锂作为下一代高能量密度电池的负极材料，具有广阔的应用前景。然而，金属锂的沉积/剥离过程常伴随着高曲折度的枝晶的形成，导致电池寿命短，甚至会诱发安全隐患。迄今为止，研究者们已开发出多种方法来抑制枝晶生长和调节固体电解质界面膜的均匀性。炭材料因其轻质、高导电、多级多孔、化学和物理稳定特性被设计成不同种类的材料来用于稳定金属锂。按照特定的功能进行分类，本文总结了炭材料在锂金属电池中作为骨架、电解液添加剂和涂层等方面的研究进展。从结构和化学方面讨论了各种炭材料的优点和局限性。最后，就如何推动锂金属电池的应用，展望了未来炭材料的发展前景。Abstract: Lithium (Li) metal is a promising anode material for next-generation high-energy-density batteries. However, the plating/stripping of Li metal is often accompanied by the formation of dendrites, which produce a short lifespan and safety hazards. To date, various approaches have been developed to suppress the dendrite growth and regulate the uniformity of the solid electrolyte interphase. Carbon materials that are lightweight, highly conductive, porous, and chemically and physically stable have been used for stabilizing the Li metal. This review summarizes the advances in carbon materials used as hosts, electrolyte additives, and coating layers in stabilizing Li metal batteries (LMBs). The advantages and limitations of various carbon materials are discussed in terms of their structural and chemical properties. Prospects for the development of carbon materials for improving LMBs are considered.
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Key words:
- Lithium metal batteries /
- Solid electrolyte interphase /
- Li dendrites /
- Inactive Li /
- Carbon materials
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Figure 1. Various carbon products for LMBs with different designs on structure, surface chemistry, functionalization, and mechanical properties.
Figure 2. (a) Schematic illustration showing the Li deposition within the Ag particle anchored CF[120]. (b-d) SEM images of Ag particle anchored CF before and after Li nucleation/growth, respectively[119]. (e, f) SEM images of pristine GT and GT after Li deposition, respectively[134]. (g) SEM image of Li/rGO composite[124]. (Reprinted with permission).
Figure 3. (a) TEM image of hollow carbon with Au nanoparticles inside. (b) Schematic illustration of Li deposition within the hollow carbon with Au nanoparticles[135]. (c) SEM image and elemental mappings of MgO modified carbonized-wood[95]. (d) SEM images of MAG before and after Li deposition along with a schematic model showing the Li/MAG interaction[139]. (e) SEM image of tubular fibers after Li deposition. Inset is the corresponding schematic diagram[138]. (f) Schematic process of creep-enabled Li deposition/stripping in a MIEC matrix. (g) SEM image of carbonaceous MIEC tubules. (h) TEM image of the Li plating process in a single carbon tubule with lithiophilic ZnOx[137]. (Reprinted with permission).
Figure 4. (a) Schematic representation of the Li nucleation on conductive frameworks[113]. (b) Schematic illustration and SEM images of Al2O3/HCS electrodes after electrochemical Li plating[143]. (c-e) Illustration of self-smoothing behavior in the Li/C anode. (f) Cycling performances of the Li/C || NMC811, Li/C || NMC622 and Li || NMC622 cells. Inset are SEM images of the flexible carbon film prepared by electrospinning, and the STEM image of an individual Li/C fiber after cycling with a smooth surface and uniform Li layer with SEI[141]. (Reprinted with permission).
Figure 5. (a) STEM and elemental mapping images of the Na, Mg, C, Mn, and F elements of a single NMMF@C cube. (b) Morphology of Li plated on the NMMF@C-modified Cu grid. (c) HRTEM image of the SEI formed on NMMF@C-modified Cu grid[142]. (d) SEM images and elemental mappings of iodine/carbon capsule. (e) SEM images of cycled Li foil without and with iodine treatment. (f) Cycling performance of Li || LiFePO4 pouch cell[140]. (Reprinted with permission).
Figure 6. (a) Time-lapse image of Li melt-infusion process for lithiophilic materials[130]. (b) Fabrication of a layered Li/rGO composite film[124]. (c) Transformation of lithium particle size during a process of chemical ethicizing and emulsification. (d) The digital photo and schematic model showing the Li microparticles dispersed in an electric and ionic dually conductive matrix composed of polymer and carbon. (e) Schematic illustration of a symmetric cell using the semi-liquid Li dispersion with improved interface contact[168]. (f) Mechanical processing of Li/C composite anode. (g) Electrochemical deposition for obtaining Li/C composite anode. (Reprinted with permission).
Figure 7. (a) Schematic illustrating the co-deposition of Li ions on nanodiamond, growth of the columnar Li film and the stripping of Li deposits. (b) Diffusion barrier of Li on different surfaces. (c) Li deposits in LiPF6-EC/DEC electrolyte with nanodiamond additives[179]. (d, e) EPMA images of cycled Li with nitro-C60 of cross-sectional morphology and C distribution, respectively. (f) HRTEM images of cycled Li with nitro-C60 additive[178]. (Reprinted with permission).
Figure 8. (a) SEM image of the hollow carbon nanosphere thin-film peeled off the Cu substrate. Inset is the SEM image of the carbon-coated polystyrene nanoparticle array. (b) Schematic illustrating the Li deposition under the protection of hollow carbon nanosphere thin-film. (c) Schematic showing the configuration of the in-situ TEM cell, and TEM images of the Li deposition process on Cu wires decorated with hollow carbon nanospheres taken at different times[189]. (d) Schematic illustrating the Li deposition in a cell using separator with a carbon-based coating layer. (e) In situ TEM images of Li deposition with the adoption of functionalized carbon[190]. (f) Schematic illustrating the double-layer nanodiamond film on a Cu substrate. (g) Cycling performance of the prototypical Li-S cells with Li foil, bare Cu with electrodeposited Li, or double-layer nanodiamond-polymer with electrodeposited Li as the anode[192]. (Reprinted with permission).
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