Recent advances in applications of graphene aerogel composite materials for electrochemical energy storage
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摘要: 石墨烯气凝胶作为一种内部互连的三维框架体，在微观和宏观尺度上具有突出的维度特性，成为各种零维、一维、二维和三维材料的理想宿主。其高导电性、高比表面积及高结构稳定性等特点令石墨烯气凝胶在储能领域得到了广泛的应用，特别是在高比容量金属离子电池负极和超级电容器电极等领域。首先，本文对石墨烯前体及气凝胶的处理策略进行整理，介绍当前不同处理方式对石墨烯前体及气凝胶成型影响。其次，根据储能机制的不同，介绍石墨烯气凝胶复合材料在主流储能器件中的改性应用及性能表现。最后，对电化学储能用石墨烯气凝胶复合材料的研究进展进行总结，指出当前存在的挑战并展望未来的研究方向。Abstract: Graphene aerogel has become an ideal host for various zero dimensional, one-dimensional, two-dimensional and three-dimensional materials because of prominent dimensional characteristics in both micro and macro scales with its interconnected three-dimensional framework. The high conductivity, specific surface area and structural stability make it widely used in the field of energy storage in recent years, especially in the application of anodes for metal ion batteries and supercapacitors electrodes with high specific capacity. Firstly, the treatment strategies of graphene precursor and aerogel are sorted out, and the effects of different treatment methods on the formation of graphene precursor and aerogel are introduced. Secondly, according to the different energy storage mechanisms, the modified application and performance of graphene aerogel composites in mainstream energy storage devices are introduced. Finally, the research progress of graphene aerogel composites for electrochemical energy storage are summarized, the current challenges are pointed out and the future research directions are prospected.
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图 1 (a) 改进Hummers制备氧化石墨烯(GO)[11]；(b) 球磨和液相剥离组合剥落石墨烯[13]；(c) 模板定向化学气相沉积法(CVD)制备石墨烯[17]
Figure 1. (a) Preparation of graphene oxide (GO) based on the modified Hummers method[11]; (b) Based on ball-milling and liquid phase exfoliated graphene[13]; (c) Graphene prepared via template-oriented chemicalvapor deposition (CVD)[17]
PVA—Polyvinyl alcohol; GNFs—Graphene nanofibers; S, S-GNFs—Stainless steel-graphene nanofibers; MFCs—Mass flow controllers
图 3 (a) 常规溶胶-凝胶法与发泡溶胶-凝胶法制备的对比图[28]；(b) 水塑发泡法制备GAs及发泡机制示意图[29]；冰晶模板法制备GA图示及孔隙结构的SEM图像(c)及冰晶成核和冰粒生长模拟图(d)[32]
Figure 3. (a) Comparative diagrams of the conventional sol-gel method and surfactant-foaming sol-gel method[28]; (b) Schematic diagram of the preparation of GAs and mechanism of hydroplastic foaming method[29]; Schematic diagram of the ice crystal template method and SEM images of porous network structures (c) and show the nucleation and anisotropy growth of ice grains (d)[32]
POM—Polarized-light optical microscopy; PRGH—Prereduced GO hydrogel; FGO—Foamed GO; GHB—Graphene hydrogel bulk
图 5 3种储能机制示意图(充电过程)
Figure 5. Schematic diagram of three energy storage mechanisms (Charging process)
图 6 MnO/多孔石墨烯气凝胶(PGA)制备示意图(a)、恒流充放电测试(b)、倍率性能(c)、循环性能(d)[54]；(e) Si@SiOx/碳纳米管(CNTs)/GA制备示意图[61]
Figure 6. Schematic diagram of preparation (a), GCD curves (b), rate performance (c) and cycling performance (d) of MnO/porous-graphene aerogel (PGA)[54]; (e) Schematic diagram of Si@SiOx/carbon nanotubes (CNTs)/GA preparation[61]
图 7 rGO@Sb2O3制备流程示意图(a)、形貌(b)和储钠倍率性能(c)[66]；(d) Sb2S3@N-C/rGO制备流程示意图[69]；(e) N、P双掺杂GA (NPGA)制备流程示意图[74]
Figure 7. Schematic illustration of the preparation procedure (a), microtopography (b) and sodium storage rate performance (c) of rGO@Sb2O3[66]; (d) Schematic illustration of the preparation of Sb2S3@N-C/rGO[69]; (e) Schematic illustration of the preparation of N, P co-doping GA (NPGA)[74]
PDA—Polydopamine
图 8 TpDq-共价有机框架(COF)/rGO气凝胶制备流程图(a)、SEM形貌(b)、充放电曲线(c)、电流密度-比容量关系图(d)[80]
Figure 8. Schematic diagram of preparation (a), SEM image (b), charge-discharge curves (c), current density-specific capacity (d) of TpDq-covalent organic frameworks (COF)/rGO aerogel[80]
PTSA—p-toluenesulfonic acid; Tp—1, 3, 5-triformylphloroglucinol; Dq—diaminoanthraquinone
图 9 聚吡咯/氧化石墨烯(PGO)@GA的结构示意图(a)、充放电曲线(b)、倍率性能(c)、EIS阻抗测试(d)、循环性能(e)[87]
Figure 9. Schematic diagram of structure (a), charge-discharge curves (b), rate performance (c) , EIS curves (d), cycling performance (e) of polypyrrole/graphene oxide (PGO)@GA[87]
Z'—Real part of impedance; Z''—Imaginary part of impedance; Rs—Solution resistance; Rct—Charge transfer resistance; W0—Warburg region; SCE—Saturated calomel electrode
图 10 TiO2−x/GA制备示意图(a)、倍率性能(b)和循环性能(c)[94]；LVO/GA的SEM和储能机制(d)、循环性能对比(e)[99]
Figure 10. Schematic illustration of preparation (a), rate performance (b) and cycling performance (c) of TiO2−x/GA[94]; SEM image and mechanism (d), cycling performance comparison (e) of LVO/GA[99]
B-TiO2−x—Black-TiO2−x; LVO—Li3VO4
表 1 锂离子电池(LIBs)用金属氧化物(MOs)-GA复合负极的MOs种类、形貌和储能性能
Table 1. MOs species, morphology and energy storage performance of metal oxides (MOs)-GA composite anode materials for lithiumion batteries (LIBs)
Anode MOs Nanomorphology Specific capacity/(mA·h·g–1) Current density/(A·g–1) Ref. Fe3O4 NWs/GA Fe3O4 Nanowires 557 2 [45] Fe3O4/GAs Nanoclusters 522.8 1 [46] Fe3O4/GA Nanoflowers 797 0.2 [47] TiO2/GA TiO2 Nanoflowers 663.2 0.1 [48] GASO SnO2 Nanoparticles 1032 0.1 [49] SnO2 NRs/GA Nanorods 1005 0.1 [50] MO/MS/SGA MoO2 Nanoparticles 533 0.5 [51] Co3O4@GA Co3O4 Nanosquares 850 0.1 [52] Notes: GASO—Graphene aerogel/SnO2; MO/MS/SGA—MoO2/MoS2/S-doped graphene aerogel; NWs—Nanowires; NRs—Nanorods. 
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表 2 超级电容器(SCs)用GA复合材料性能表现
Table 2. Energy storage performance of GA composite materials for supercapacitors (SCs)
Electrode material Specific capacity Cycle performance Ref. All SCs Bio-AC/rGO/CNF//MnO2/Bio-AC/rGO/CNF 812 mF·cm–2 99% capacitance retention after 5000 cycles [78] ETAC/CNF/rGO 556 F·g–1 97.5% capacitance retention after 10000 cycles [79] TpDq-COF/rGO 269 F·g–1 96% capacitance retention after 5000 cycles [80] DAAQ-COFs/GA 378 F·g–1 88.9% capacitance retention after 20000 cycles [81] v-COF-GAs 289 F·g–1 92% capacitance retention after 20000 cycles [82] All SCs PPys-CNTs@3D//GA MnO2@CNTs@3D GA 950 mF·cm–2 84.6% capacitance retention after 2000 cycles [83] PANI/rGO 808 F·g–1 73% capacitance retention after 1000 cycles [84] GA-Fe2O3 200 F·g–1 72.3% capacitance retention after 5000 cycles [85] MnO2/GA 275 F·g–1 100% capacitance retention after 5000 cycles [86] Notes: Bio-AC—Biomass active carbon; CNF—Cellulose nanofiber; ETAC—Eucommia wood tar-based activated carbon; TpDq—1, 3, 5-triformylphloroglucinol diaminoanthraquinone; COF—Covalent organic frameworks; DAAQ—2, 6-diaminoanthraquinone; PPy—Polypyrroles; PANI—Polyaniline.
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