Three-dimensional printed carbon-based microbatteries: progress on technologies, materials and applications
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摘要: 可充电微型电池可以为下一代可穿戴便携设备提供储能装置。增材制造也称为三维(3D)打印技术,具有构建复杂3D构型的能力,为制备尺寸可调、形状一致性好、兼具高能量密度和高功率密度的微电池提供了新的机遇。与其他多孔金属电极材料相比,轻质炭材料具有比表面积大、导电性好、化学稳定性高等优点。近年来,基于碳基墨水的3D打印技术已被用于制备多种类型的可充电微电池。为了对碳基微电池的电化学性能进行优化,并充分发挥其潜力,亟需对3D打印技术、材料设计以及应用方向进行梳理,从而深入理解3D打印电池方法的设计优化策略。本文首先介绍了4种主要3D打印技术的最新进展,阐述了导电炭材料在解决3D打印微电池挑战中的研究方法,总结了其在一系列储能设备和可穿戴电子设备集成中的应用。最后,进一步讨论了3D打印技术制造碳基微电池面临的关键科学问题和未来的发展方向。Abstract: Next-generation wearable and portable devices require rechargeable microbatteries to provide energy storage. Three-dimensional (3D) printing, with its ability to build geometrically complex 3D structures, enables the manufacture of microbatteries of different sizes and shapes, and with high energy and power densities. Lightweight carbon materials have a great advantage over other porous metals as electrode materials for rechargeable batteries, because of their large specific surface area, superior electrical conductivity and high chemical stability. In recent years, a variety of rechargeable microbatteries of different types have been successfully printed using carbon-based inks. To optimize their electrochemical performance and extend their potential applications, it is important to analyze the design principles with respect to the 3D printing technique, printable carbon materials and promising applications. This paper provides a perspective on recent progress in the four major 3D printing techniques, elaborates on conductive carbon materials in addressing the challenging issues of 3D printed microbatteries, and summarizes their applications in a number of energy storage devices that integrate with wearable electronics. Current challenges and future opportunities for carbon-based microbattery fabrication by 3D printing techniques are discussed.
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Key words:
- 3D printing /
- Microbattery /
- Carbon materials /
- Graphene
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Figure 2. (a) Conventional battery geometries. (b) 3D designed microbatteries with interdigitated anode and cathode plate configuration[35]. Reprinted with permission.
Figure 3. Schematic diagram of (a) the direct ink printing (DIW) technique, (b) fused deposition modeling (FDM) technique, (c) selective laser sintering (SLS) technique, (d) stereolithography (SLA) technique and (e) material jetting technique (e)[40]. Reprinted with permission.
Figure 4. (a) Digital image displaying the procedure of printing the 3D architectures line-by-line (upper), and isometric view of the holey graphene oxide (hGO) mesh with a 0.8 mm line spacing (bottom)[54]. (b) Schematic illustration of the 3D printing process for sulfur/carbon black thick cathodes (10 mm grid diameter)[31]. (c) Schematic of synthesis of 3D graphene foams (GFs)[61]. (d) Designed structure of C-MEMS 3D microbattery[62]. Reprinted with permission.
Figure 5. (a) Schematic illustration of the 3D printed negative electrode disc (graphite/PLA) elaboration process[50]. (b) Digital photo of the 3D printing process of graphene/PLA filament. (c) Schematic of the coin cell fabrication with the graphene/PLA anode. (d) Coulombic efficiency of the 3D printed graphene/PLA anode. (e) Rate capability of the 3D printed graphene/PLA anode[47]. Reprinted with permission.
Figure 6. (a) Model of the 3D-printed graphene-based electrodes. The external walls are the current collector (Cu), and the internal walls are graphene. (b) Digital image of the chemically modified graphene (CMG)/Cu one-leg component after freeze-drying. (c) SEM images of the interface of reduced chemically modified graphene (rCMG)/Cu. (d) SEM images inside the rCMG filaments[36]. (e) Digital image of a miniaturized version of the 3D-printed LFP/rGO and LTO/rGO electrodes. (f) Digital photo of the 3D-printed LFP/rGO and LTO/rGO electrode arrays. (g) Charge and discharge curves of the LFP/rGO half-cell at a current density of 10 mA g−1. Inset is a schematic of the planar battery. (h) Charging and discharging curves of the full cell[19]. Reprinted with permission.
Figure 7. (a) Schematic diagram of the IJP setup. (b-c) Schematic diagram of the 3D printed ATM/GO composite droplets. (d) Formation of ice crystal during 3D printing. (e) ATM/GO composite aerogel after freeze drying. (f) Image of the ATM/GO aerogel after freeze drying. (g) Image of the ATM/GO aerogel after annealing[9]. (h) SEM image of the yarn composed of three LFP fibers. (i) Schematic diagram of the all-fiber LIB device[69]. (k) Schematic diagram of the 3D-printed full cell[39]. Reprinted with permission.
Figure 8. (a) Schematic illustration of 3DP-Air-electrode. (b) Schematic illustration of the reaction region of the Zn-O2 battery. The double green balls represent oxygen molecules[26]. (c) Schematic illustration of the Ni/r-GO framework. (d) Low-magnification FESEM image of the Ni/r-GO electrode. (e) Discharge and charge curves of the Ni/r-GO cathode at a current density of 100 mA g−1. (f) Discharge and charge curves of the Ni/r-GO cathode at various current densities with a capacity limit of 1000 mA h g−1[24]. Reprinted with permission.
Figure 9. (a) Independent components of the 3D printed coin cell. (b) Assembled coin cell. (c) 3D printed glasses with a LCD lens and 3D printed batteries integrated. (d) Digital photos showing the sunglasses transmitting and blocking the image of the Duke Chapel with LCD off and on, respectively. (e) Separated components of a 3D printed bangle battery integrated with LED. (f) LED powered by the 3D printed bangle battery[74]. (g) Prototype photo of the printed battery before being integrated into the textile and (h) after being integrated into the biomonitoring belt to provide 22 h autonomy[91]. Reprinted with permission.
Table 1. A comparison of different 3D-printing techniques.
3D printing techniques Inks Macroporosity Fraction of active materials Resolution (μm) Strengths Weaknesses Direct ink writing (DIW) Metal, ceramic, or polymer gels with high viscosity, suitable rheological and viscoelastic properties 5–10 μm[41]
~200 μm[23,30]
300–400 μm[42]0.06–0.43 (v/v)[41]
70%[19]1–100 Versatile easy operation Required post-processing Low resolution Fused deposition modeling (FDM) Thermoplastic filaments with active materials ~500 μm[34] 8%[47] 50–200 Low cost Single material Selective laser sintering (SLS) Metal, polymer or ceramic powders 0.0012–
0.0071 mm3[43]5%–40%[45] 80–250 Simple material processing High cost Stereolitho-graphy (SLA) Photosensitive liquid resin consisting of active materials, photoinitiators, and prepolymers with good flowability and suitable refractive index ~300 μm[46] 0.08%–
0.20%[41]>10 High resolution and efficiency good surface quality Limited to photocurable materials required solvents (resins) Inkjet printing (IJP) Low viscosity Newtonian
liquid (40–100 cP)65%–70%[51] 70%[9] 5–200 High flexibility of multi-material capability Lack of self-standing ability, low printing speed Table 2. Electrochemical performance over a series of 3D printed carbon-based microbatteries.
Printed carbon-based component 3D-printing
techniqueAnode/Cathode Battery type Electrochemical performance Si/C-graphite[93] DIW [Si/C-graphite]/Li Li-ion battery 484 mA·h g−1 (C/4) Graphite/PLA[50] FDM [graphite/PLA]/Li Li-ion battery 200 mAh·g−1 (cathode) at 18.6 mA·g−1 (C/20) Graphite/PLA and LFP/carbon black[33] FDM [graphite/PLA]/[LFP/carbon black] Li-ion battery 165 mAh·g−1 (anode) at 10 mA·g−1 rGO-AgNWs-LTO[94] DIW Li/rGO-AgNWs-LTO Li-ion battery 121 mAh·g−1 (10 C)
4.74 mAh·cm−2LFP/GO, LTO/GO[19] DIW [LTO/GO]/[LFP/GO] Li-ion battery ~160 mAh·g −1 (cathode)
and ~170 mAh·g −1 (anode) at 10 mA·g−1Graphene/PLA[48] FDM [graphite/PLA]/Li Li-ion battery 500 mAh·g-1 at 40 mA·g-1 (anode) PoPD/nanocarbon/LMO[29] FDM Pt/[PoPD/nanocarbon/LMO] Li-ion battery 69.1 mAh·g−1 at 0.036 mA·cm−2 (cathode) LFP/CNTs[34] FDM Li/[LFP/CNTs] Li-ion battery 7.5 mAh·cm−2 (cathode)
69.41 J·cm−2 at
2.99 mW·cm−2LTO/CNTs, LFP/CNTs[39] DIW [LTO/CNTs]/[LFP/CNTs] Li-ion battery ~110 mAh·g−1 at 50 mA·g−1 LiNi0.8Co0.15Al0.05O2/CF, CF[32] DIW CF/[LiNi0.8Co0.15Al0.05O2/CF] Li-ion battery 191 mAh·g−1 (0.1 C) LTO/Graphene, LMO/MWCNT[74] FDM [LTO/Graphene]/[LMO/MWCNT] Li-ion battery 3.91 mAh·cm–3, coulombic Sulfur/DIB/GO[42] DIW&FDM Sulfur/[Sulfur/DIB/GO] Li-S battery 812.8 mAh·g−1 at 50 mA·g−1 aMWCNT[64] IJP Li/aMWCNT Li-S battery ~7 mAh·cm−2 at 11.5 mA·cm−2 S@SWCNTs[65] IJP Li/[S@SWCNTs] Li-S battery 850 mAh·g–1 (C/2), between 700 and
800 mAh·g–1 for 100 cycles (C/2)S/C composite[95] DIW Li/[S/C composite] Li-S battery 530 mAh·g−1 at 10 mA·cm−2 LaB6/C@S[96] DIW Li/[LaB6/C@S] Li-S battery 693 mAh·g−1 S/C[31] DIW Li/[S/C] Li-S battery 1009 mAh·g−1 Li/CNTs, Se[27] DIW [Li/CNTs]/Se Li-Se battery 12.99 mAh·cm−2 at 3 mA·cm−2 Li-plated 3DP-NC[30] DIW [Li-plated 3DP-NC]/LiFePO4 Li-metal battery 30 mAh·cm–2 at 10 mA·cm–2 hGO meshes[54] DIW Li/hGO Li-O2 battery 13.3 mAh·cm−2 at 0.1 mA·cm−2 (cathode)
(~4.8 mA·h or ~3879 mAh·g−1 in total capacity)Co/N-doped carbon[23] DIW Li/[Co/N-doped carbon flakes] Li-O2 battery Energy density of 798 Wh·kg–1 cell Ni-rGO[24] DIW Li/[Ni-rGO] Li-CO2 battery 14.6 mAh·cm–2 at 0.1 mA·cm–2
(8991.0 mAh·g–1)rGO/Na3V2(PO4)3[12] DIW rGO/Na3V2(PO4)3 Na-ion battery 1.26 mAh·cm–2 (0.2 C) (cathode)
0.39 mAh·cm–2 (1 C) (full cell)MoS2/rGO[9] IJP [MoS2/rGO]/Na Na-ion battery 429 mAh·g−1 at 100 mA·g−1 (~ C/3.3) rGO[28] DIW CP-protected Na/rGO Na-O2 battery 13484.6 mAh·g−1 at 0.2 A g−1 Zn/CB/CF, MnO2/GO/CNTs[26] DIW [Zn/CB/CF]/[MnO2/GO/CNTs] Zn-O2 battery 670 mAh·g–1 at 5 mA·cm–2 Ag2O-SIS, Ga-CB-SIS[91] DIW Ga-CB-SIS/Ag2O-SIS Ag-Ga battery ~19.4 mAh·cm−2 -
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