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摘要: 凭借着钠资源储量丰富和成本优势，钠离子电池在电化学储能领域有望成为锂离子电池的重要补充。作为钠离子电池负极材料，炭及其复合材料可以通过合理的结构设计和组分调控获得优异的储钠性能。随着可穿戴电子器件日益普及，人们对电极提出了更高的性能要求。自支撑电极无需使用电化学惰性的黏结剂和导电添加剂等组分，有利于提升电池体系能量密度。本文总结了近年来钠离子电池用自支撑炭基电极材料的最新研究进展，包括碳纳米纤维、碳纳米管、石墨烯及其复合材料，从基底有无的角度详细综述并讨论了自支撑炭基负极的制备策略及其电化学性能，最后对钠离子电池用自支撑炭基负极材料的未来挑战和发展进行了展望。Abstract: Sodium-ion batteries (SIBs) have received extensive research interest as an important alternative to lithium-ion batteries in the electrochemical energy storage field by virtue of the abundant reserves and low-cost of sodium. In the past few years, carbon and its composite materials used as anode materials have shown excellent sodium storage properties through structural design and composition regulation. The increasing popularity of wearable electronics has demanded higher requirements for electrode materials. A free-standing electrode is able to eliminate the massive use of electrochemical inactive binders and conductive additives, thereby increasing the overall energy density of the battery system. Research progress on carbon materials such as carbon nanofibers, carbon nanotubes and graphene and their composites (metallic compounds and alloy-type materials) is summarized. The preparation strategies and electrochemical properties of free-standing carbon-based anodes with and without substrates are categorized and reviewed. Finally, proposals are made for future research and developments for free-standing carbon-based anodes for SIBs.
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Figure 2. Schematic diagram of Na storage mechanisms: (a) carbonaceous materials, (b) alloy materials, and (c) metallic compounds
Figure 3. (a) Schematic illustration of the fabrication for porous CNFs. (b) Na-ion diffusion mechanism of freestanding porous CNFs electrode. Reproduced with permission[41]. Copyright 2014, Royal Society of Chemistry. (c) Schematic of the preparation for N-doped CNFs. (d) Rate capability of N-doped CNFs. Reproduced with permission[42]. Copyright 2016, Wiley–VCH. (e) Schematic illustration of the synthesis for P-doped CFs. (f) Slope and plateau capacity comparison of CNFs and P-doped CNFs. Reproduced with permission[43]. Copyright 2018, American Chemical Society
Figure 4. (a) TEM image of FeP@NPC. (Inset shows flexibility of FeP@NPC film.) (b) Cycling performance of FeP@NPC electrode at 1 A g−1. Reproduced with permission[55]. Copyright 2020, Elsevier. (c) Schematic of the preparation process for CoTe2@NMCNFs. (d) SEM image of CoTe2@NMCNFs. (e) N2 adsorption–desorption isotherms of CoTe2@NMCNFs and CoTe2@NCNFs. Reproduced with permission[56]. Copyright 2021, American Chemical Society. (f) Schematic illustration of the preparation for Sn NDs@PNC nanofibers. (g) Digital photos of electrospinning product before and after calcination. (h) Electrochemical performance of Sn NDs@PNC with different Sn contents. (Inset shows the HRTEM of Sn dots before and after cycling.) Reproduced with permission[32]. Copyright 2015, Wiley-VCH
Figure 5. (a) Schematic illustration of the preparation for NCP@FCNT-FS film. (b) SEM image of 2D Ni1.5Co0.5Px nanosheets. (c) Digital image of the bending film. (d) Rate capacities of NCP/C, NCP/CNT, and NCP@FCNT-FS. Reproduced with permission[64]. Copyright 2018, Wiley–VCH. (e) Schematic illustration of construction for Fe1−xS@PCNWs/rGO paper. (f) Digital images for various deformations, (g) SEM images, and (h) cycling stabilities for different mass loading of Fe1−xS@PCNWs/rGO. Reproduced with permission[65]. Copyright 2019, Wiley–VCH. (i) Schematic illustration of preparation for P@NGCA. (j) Compressive stress–strain curves and (k) electronic conductivity of GA, GCA, and NGCA. (l) Cycling performance of P@NGCA. Reproduced with permission[69]. Copyright 2022, Royal Society of Chemistry
Figure 6. (a) Schematic of the preparation process for 1T-MoS2/CC. SEM image of (b) MoO3/CC and (c) 1T-MoS2/CC. Reproduced with permission[79]. Copyright 2018, Royal Society of Chemistry. (d) Model diagram, (e) SEM image of CoxP@CFC, and (f) P 2p XPS analysis of CoxP@CFC. (g) TEM image of mixed-valence CoxP. (h) Comparison of cycling performance at 0.1 A g−1. Reproduced with permission[82]. Copyright 2022, Wiley–VCH. (i) Schematic diagram of the morphology change and (j) Na+ diffusion coefficient comparison of CoP@PPy NWs/CP and CoP NWs/CP during cycling processes. Reproduced with permission[85]. Copyright 2018, Wiley–VCH
Figure 7. (a) Digital photographs and schematic diagram of preparation for MFCPs. (b) HRTEM of MFCP-1300. (c) ICE and (d) slope/plateau capacity of a series of MFCPs at 20 mA g−1. Reproduced with permission[92]. Copyright 2021, Elsevier. (e) Schematic of the preparation process for MoS2@CSC. (f) Top and sectional SEM images and (g) Rate performance of MoS2@CSC. Reproduced with permission[93]. Copyright 2019, American Chemical Society. (h) Schematic diagram of 3D carbon-networks/Fe7S8/graphene. (i) SEM image and flexibility display of CFG. (j) Na storage performance of CFG. Reproduced with permission[94]. Copyright 2019, Wiley–VCH
Table 1. The reported synthetic methods and electrochemical properties of free-standing carbon-based anodes for SIBs
Substrate Materials Synthetic methods ICE Electrochemical performance Ref. Free Porous CNFs Soft template and electrospinning 53.5% 266 mAh g−1@0.05 A g−1 after 100 cycles [41] N-doped CNFs Electrospinning - 377 mAh g−1@0.1 A g−1 after 100 cycles [42] N/S co-doped CNFs Electrospinning 62.0% 336 mAh g−1@0.05 A g−1 after 100 cycles [48] P-doped CNFs Electrospinning 55.7% 253 mAh g−1@0.05 A g−1 after 200 cycles [43] FeP@NPC Electrospinning and phosphatization 49.0% 391 mAh g−1@0.1 A g−1 after 1000 cycles [55] CoTe2@NMCNFs Electrospinning and tellurization 57.1% 261.2 mAh g−1@0.2 A g−1 after 300 cycles [56] Sn NDs@PNC Electrospinning 70.0% 483 mAh g−1@2 A g−1 after 1300 cycles [32] P/CFs@RGO Electrospinning and vaporization condensation 73.8% 406.6 mAh g−1@1 A g−1 after 180 cycles [57] Sn/CFC Electrospinning 42.3% 255 mAh g−1@0.05 A g−1 after 200 cycles [58] Bi/CNFs Electrospinning 53.0% 186 mAh g−1@0.05 A g−1 after 100 cycles [59] SbNP@C Electrospinning 55.5% 350 mAh g−1@0.1 A g−1 after 300 cycles [60] NCP@FCNT-FS Phosphatization and vacuum filtration - 196.6 mAh g−1@0.5 C after 100 cycles [64] Fe1−xS@PCNWs/rGO Vacuum filtration and sulfuration 66.2% 573 mAh g−1@0.1 A g−1 after 100 cycles [65] P@NGCA Freeze-drying and vaporization condensation 80.0% 538 mAh g−1@0.2 A g−1 after 100 cycles [69] NS-C film Vapor phase polymerization - 379.1 mAh g−1@0.1 A g−1 after 1000 cycles [73] CC 1T-MoS2/CC Hydrothermal and sulfuration 77.7% 576 mAh g−1@0.2 A g−1 after 200 cycles [79] CC SnS2@graphene nanosheet Hydrothermal 57.4% 378 mAh g−1@1.2 A g−1 after 200 cycles [80] CC CoxP@CFC Hydrothermal and phosphatization 69.4% 814 mAh g−1@0.1 A g−1 after 100 cycles [82] CC Sb2O3/CC Solvothermal 84.5% 900 mAh g−1@0.05 A g−1 after 100 cycles [83] CP CoP@PPy NWs/CP Hydrothermal, phosphization, and polymerization 69.1% 0.521 mAh cm−2@0.15 mA cm−2 after 100 cycles [85] CP MoS2@C Hydrothermal and calcintion 79.4% 286 mAh g−1@0.08 A g−1 after 100 cycles [87] CP 3D Sn@CNT-CP Freezing-drying and chemical vapourdeposition 81.7% 0.455 mAh cm−2@0.25 mA cm−2 after 100 cycles [86] CF CoP4/CF Hydrothermal and phosphatization - 851 mAh g−1@0.3 A g−1 after 300 cycles [88] Cotton CFG Vacuum drying and calcintion 81.0% 0.75 mAh cm−2@6 mA cm−2 after 5000 cycles [94] Cotton HCF-V2O5 Hydrothermal 69.4% 184 mAh g−1@0.05 A g−1 after 100 cycles [95] Silk N-SWC/SnOx@rGO Freezing-drying and calcintion 84.1% 572.2 mAh g−1@0.1 A g−1 after 100 cycles [96] Ni foam NC/NF Hydrothermal reactions 63.1% 225.4 mAh g−1@5 A g−1 after 1000 cycles [97] Ni foam Ni2P/3DG Chemical vapor deposition and hydrothermal reactions 88.3% 212.4 mAh g−1@0.1 A g−1 after 200 cycles [98] 
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