Electrohydrodynamic 3D printing of orderly carbon/nickel composite network as supercapacitor electrodes

doi:10.1016/j.jmst.2020.12.034

Abstract

Abstract:

Electrohydrodynamic (EHD) 3D printing of carbon-based materials in the form of orderly networks can have various applications. In this work, microscale carbon/nickel (C-Ni) composite electrodes with controlled porosity have been utilized in electrochemical energy storage of supercapacitors. Polyacrylonitrile (PAN) was chosen as the basic material for its excellent carbonization performance and EHD printing property. Nickel nitrate (Ni(NO₃)₂) was incorporated to form Ni nanoparticles which can improve the conductivity and the capacitance performance of the electrode. Well-aligned PAN-Ni(NO₃)₂ composite structures have been fabricated and carbonized as C-Ni electrodes with the typical diameter of 9.2±2.1 μm. The porosity of the as-prepared C-Ni electrode can be controlled during the EHD process. Electrochemical results show the C-Ni network electrode has achieved a 2.3 times higher areal specific capacitance and 1.7 times higher mass specific capacitance than those of a spin-coated electrode. As such, this process offers a facile and scalable strategy for the fabrication of orderly carbon-based conductive structures for various applications such as energy storage devices and printable electronics.

Key words: Electrohydrodynamic 3D printing, Carbon-nickel structure, Controlled porosity, Supercapacitors

Bing Zhang, Jiankang He, Gaofeng Zheng, Yuanyuan Huang, Chaohung Wang, Peisheng He, Fanping Sui, Lingchao Meng, Liwei Lin. Electrohydrodynamic 3D printing of orderly carbon/nickel composite network as supercapacitor electrodes[J]. J. Mater. Sci. Technol., 2021, 82: 135-143.

Figures/Tables 8

Fig. 1. Schematic illustration of the EHD 3D printing and carbonization process for C-Ni composite electrodes.

Fig. 2. Investigation of the processing parameters in EHD printing. (a) Graphical illustration of the working mechanism of EHD printing. (b) Optical image of EHD-printed fibers with different width. (c-f) Experimental results showing the EHD-printed PAN-Ni(NO3)2 fiber width with respect to (c) applied voltage, (d) nozzle-to-collector distance, (e) feeding rate, and (f) stage moving speed. The standard EHD printing process includes: applied voltage of 1400 V, nozzle-to-collector distance of 3 mm, feeding rate of 20 μL h-1 and stage moving speed of 50 mm s-1. Only one parameter was altered for each group.

Fig. 3. EHD 3D printing of the PAN-Ni(NO3)2 networks. (a) Schematic diagram of EHD-printed 3D structures with 10 to 50 layers. (b) 3D profiles of the printed structures obtained from laser confocal scanning. (c) The structural height with respect to the number of layers. (d) Optical images of the 50-layer lattice structure with a 500 μm gap spacing.

Fig. 4. SEM images of the C-Ni 3D structures (a) before and (b) after carbonization.

Table 1 Comparison of conventional 3D printing techniques for carbon-based materials.

3D printing process	Materials	Resolution (μm)	Refs.
Fused deposition molding	Carbon fiber powder, ABS thermoplastic pellet	200	[44]
Direct ink writing	PLA-MWCNTs ink	100	[45]
Projection microstereolithography	Photosensitive resin, Chopped carbon fiber	50	[46]
Selective laser sintering	Phenolic resin, Carbon fiber powder	500	[47]
Selective laser melting	Carbon nanotube, Al-Si10Mg powder	80	[48]
EHD 3D printing	PAN-Ni₂(NO)₃ ink	9.2 ± 2.1	This work

Fig. 5. Materials characterization of the EHD-printed PAN-Ni(NO3)2 structure and the C-Ni electrode. (a, b) EDS spectrum of the PAN-Ni(NO3)2 structure and C-Ni electrode. (c) XRD spectrum of the C-Ni electrode. (d) Raman spectrum of the C-Ni electrode. (e) EDS elemental mapping of C, O and Ni for the C-Ni electrode.

Fig. 6. Electrochemical and structural properties of the C-Ni electrodes. (a) CV curves of the C-Ni electrodes with the printed fiber spacing of 20, 40, 60, 80, 100 and 120 μm, at the scanning rate of 10 mV s-1. (b) CV curves of the EHD-printed electrodes and spin-coated electrodes, at the scanning rate of 10 mV s-1. (c) The mass specific capacitances of the EHD-printed and spin-coated electrodes. (d) The conductivity and porosity of the EHD-printed electrodes.

Fig. 7. Electrochemical performance of the as-fabricated C-Ni electrodes. (a) CV curves of the 60 μm-spacing sample at the scanning rates of 10, 20, 50 and 100 mV s-1. (b) GCD curves of the 60 μm-spacing sample with the current density of 1, 2, 3, 4 and 5 mA cm-2. (c) Nyquist plot of the EHD-printed samples with varied fiber spacing of 20, 40, 60, 80, 100 and 120 μm. (d) The cycling stability test of the 60-μm spacing sample at the scanning rate of 100 mV s-1. Inset: CV curves at the first cycle, after 500 and 5000 cycles.

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