A comprehensive review of the 3D printing of sp2 carbons: Materials, properties and applications
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摘要:
3D打印可以改变现有的生产方法，是第四次工程革命中的一项现代技术。它从成型原理上提出了分层制造、逐层叠加成型的新颖生产方法，从根本上简化了制造工艺，实现了大规模定制生产。然而，这一新技术仍存在许多问题。除了纯石墨烯外，sp2碳具有好的亲水性，3D打印难度较小。sp2碳还可在3D打印中的各种阶段应用。纯石墨烯的疏水性使其难以在水系介质中打印和加工。毛细管油墨的发展使得纯石墨烯的3D打印成为可能。本文综述了sp2碳的3D打印技术的最新进展。首先简要概述了3D打印技术，随后概述了sp2碳的3D打印及其在各种方面的应用。最后，讨论了这一新领域的发展前景和机遇。
Abstract:Three dimensional (3D) printing is a modern technology that has the possibility to transform existing production methods. It offers a novel production method of layered manufacturing and layer-by-layer stacking, which radically simplifies the manufacturing process and enables large-scale customizable production. However, there are still numerous problems with this new technology. Except for pure graphene, sp2 carbons can be 3D printed with little difficulty because of their hydrophilicity. The hydrophobic nature of pure graphene makes it difficult to print and process in water-based media, but advances in capillary inks allow for the 3D printing of pure graphene. This review focuses on the most recent developments in the 3D printing of sp2 carbons. A concise overview of 3D printing technologies is presented, followed by a summary of 3D printed sp2 carbons and their diverse applications. Finally, prospects and opportunities for this new field are discussed.
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Key words:
- 3D printing technologies /
- sp2 carbons /
- Carbon-based composites /
- Applications
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Figure 1. Schematic representation of 3D printed sp2 carbons and their possible applications
Figure 2. Technical classification of 3D printing techniques. PolyJet: photopolymer jetting, SLM: selective laser melting, HSS: high-speed sintering, BJ: binder jetting, EBM: electron beam melting. Adopted from Ref.[45] with little modifications
Figure 3. Cyclic voltammetric (CV) of (a) TBHQ, (b) BHA, (c) differential pulse voltammetry responses of TBHQ and BHA, and (d) corresponding calibration curves. Reproduced from Ref.[59] with permission from Springer. (e) Calculated reflection loss curves, (g) corresponding 3D plot, (f) layer thickness matching , and (h) effective absorption bandwidth. Reproduced from Ref.[57] with permission from the Elsevier
Figure 4. (a) SEM image of 3D printed CNTs. (b) Schematic of fabricated device. (c) Real-time digital image of the device. (d) CV profile of 3D printed CNT device. Reproduced from Ref.[72] with permission from the American Chemical Society. (e) TEM image of CNTs. (f) Schematic of the device in which polymer gel electrolyte is cast. (g) SEM image of the electrode material. (h) CV profile of packaged device. Reproduced from Ref.[73] with permission from the American Chemical Society
Figure 5. (a) and (c) Printed structures. (b) and (d) FESEM images. (e) Viscoelastic fingerprints of 3D printed PVA-GO ink with 0.3% GO loading. Reproduced from Ref. [99] with permission from the American Chemical Society
Figure 6. (a) Graphical representation of printing process and different structures printed with GO/geopolymer nanocomposite. (b) Printability of GG/GO bio-inks. Digital images of (c) the printed matrix pentagram, (d) gradient spacing grids and ( e, f, g) printing fidelity for GO bio-inks. Reproduced from Ref.[102] and [92] with permission from the Elsevier
Figure 7. (a) Schematic of 3D rGO scaffold preparation. (b) Macroscopic images of prepared scaffolds (side and top views). (c) Biological properties. Reproduced from Ref.[100] with permission from the Elsevier
Figure 8. (a) Schematic of temperature treatment setup for rGO. (b) Digital image of Al-rGO thin film. I vs V profile of Al-rGO film (c) before and (d) after heat treatment. (e) Al-rGO thin film under Joule heating. (f) Emission spectra of thin-film. (g) Temperature monitored at different powers. (h) Raman spectra with and without heat treatment. Reproduced from Ref.[101] with permission from Nature
Figure 9. (a) Graphical representation of ink formulation and printing. (b) Conductivity of 3D printed aqueous graphene ink. (c) Storage modulus vs octanol amount. X-ray tomography analysis: (d) 3D image, (e) cross-section view and (f) histogram of graphene flake orientation. Reproduced from Ref.[117] with permission from the Royal Society of Chemistry. (g) Digital image and schematic of 3D printed device. (h) CV profile, (i) GCD profile, (j) histogram of areal capacitance, (k) cycle test profile and (l) Nyquist plot ofthe 3D printed flexible supercapacitor. Reproduced from Ref.[118] with permission from the American Chemical Society
Figure 10. (a) Schematic and optical micrographs of the graphene electrode. (b) and (c) The morphology of printed graphene electrode. (d) 2D and 3D images for surface roughness study. (e) and (f) AFM image and height profile of the electrode. (g) The electrode thickness vs printing speed. (h) Conductivity vs electrode thickness. (i) Resistance vs electrode length. (j) CV profile, (k) Nyquist plot and (l) magnified Nyquist plot for the annealed electrode. Reproduced from Ref.[120] with permission from the American Chemical Society
Figure 11. (a) Schematic mechanism of self-healing and shear-thinning behavior of colloidal gel. (b) SEM and (c) digital image of a colloidal gel. Reproduced from Ref.[122] with permission from the Royal Society of Chemistry. (d) 3D printed GQDs structure. (e) and (f) Fluorescence images at 365 nm excitation. (g) Storage (solid) and loss (empty) modulus curves of GQD-hydrogel. (h) Effect of cycling on storage and loss modulus. Reproduced from Ref.[127] with permission from the American Chemical Society
Table 2. 3D printed sp2 carbons and their applications
Materials Applications Ref. Graphene-CMC Electrical properties [117] Graphene-aerogel Energy storage [141] Graphene/Li0.35Zn0.3Fe2.35O4 Microwave absorption [142] Graphene/Carbonyl Iron/PMMA Microwave absorption [143] Graphene-polyamide Electric motor [144] GO-LFP and GO-LTO Energy storage [145] Functionalized-GO Biosensors [146] GO-PLA Bone tissue engineering [147] rGO-polycaprolactone Regenerative engineering [148] rGO/magnesium nanohybrid Bone tissue engineering [149] rGO-polycaprolactone Antibacterial and Tissue Engineering [150] rGO-gold composite Electrochemical detection [151] rGO-MXene Electromagnetic interference shielding [152] rGO-MnO2 Energy storage [153] GO-elastomer resin composite Strain sensors [154] CNT yarn-Ultem Structural applications [155] Multiwall CNTs-PLA Conductive patterns [156] CNTs-PLA Welding [157] CNTs-Polycaprolactone Cardiac Tissue Engineering [158] Multiwall CNTs-PEGDA bioink Nerve regeneration [159] CNTs-TPU Multiaxial force sensors [160] Multiwall CNTs-PDMS Strain sensors [161] Orange CDs-sodium polyacrylate Optical properties [133] CDs-hydrogels Optical properties [162] Red CDs-2-HCA Gas sensors [163] 
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