Three-dimensional Au/carbon nanotube-graphene foam hybrid nanostructure for dendrite free sodium metal anode with long cycle stability

doi:10.1016/j.jmst.2022.01.003

Abstract

Abstract:

Sodium metal anode has been attracting widely research attention due to its large capacity and low electrode potential as the anode of sodium-ion batteries. However, the uncontrollable growth of Na dendrite is one of the critical issues for its real applications. Herein, a three-dimensional (3D) nanostructure composed of gold nanoparticles (Au NPs) supported on 3D carbon nanotube-graphene foam (3D CNT-GF) was designed and fabricated as the host of sodium metal anode. Na@3D Au/CNT-GF anode can deliver a Coulombic efficiency of 99.14% and stably cycle for 2600 h at 1 mA cm^-2 with 1 mAh cm^-2. It can cycle for 300 h at 5 mA cm^-2 with 1 mAh cm^-2. Detailed results indicate that its excellent electrochemical performance can be attributed to the unique macroporous structure and sodiophilic surface formed by Au NPs guiding the uniform sodium metal deposition enabled a dendrite-free morphology investigated by the ex-situ SEM and in-situ optical microscopy. At last, a full cell was assembled with Na@3D Au/CNT-GF as the anode and Na₃V₂(PO₄)₃@C as the cathode. It can deliver a capacity of 84.6 mAh g^-1 at 100 mA g^-1 after 200 cycles. Our results demonstrate that 3D Au/CNT-GF is a promising sodium metal anode host.

Key words: 3D Au/CNT-GF, Sodiophilic Au NPs, Dendrite free, Uniform deposition, In-situ optical microscopy investigation

Zhenxin Huang, Zixuan Wang, Bofang Tian, Tingting Xu, Caiyun Ma, Zhuangfei Zhang, Jinhao Zang, Dezhi Kong, Xinjian Li, Ye Wang. Three-dimensional Au/carbon nanotube-graphene foam hybrid nanostructure for dendrite free sodium metal anode with long cycle stability[J]. J. Mater. Sci. Technol., 2022, 118: 199-207.

Figures/Tables 7

Fig. 1. (a) Schematic diagram of the preparation process of 3D Au/CNT-GF nanostructure. (b-d) SEM images of 3D Au/CNT-GF at different magnifications. Inset in (b) is a digital image to show the flexibility of 3D Au/CNT-GF nanostructure. (e, f) TEM and (g) HRTEM images of 3D Au/CNT-GF nanostructures. (h) SEM image of 3D Au/CNT-GF nanostructure. (i, j) Corresponding EDS element mapping of Au and C, respectively.

Fig. 2. (a) XRD patterns and (b) Raman spectra of 3D Au/CNT-GF and 3D CNT-GF nanostructure, and (c) TGA curve of 3D Au/CNT-GF nanostructures.

Fig. 3. The current density distribution on (a) Cu, (b) 3D CNT-GF and (c) 3D Au/CNT-GF electrodes simulated by COMSOL Multiphysics. In-situ optical photos of Na deposition on (d) Cu, (e) 3D CNT-GF and (f) 3D Au/CNT-GF taken by a digital camera. The scale bars in (d-f) are 400 µm. Schematic diagrams of Na metal deposition on (g) Cu, (h) 3D CNT-GF and (i) 3D Au/CNT-GF electrodes.

Fig. 4. Electrochemical performance of Cu, 3D CNT-GF and 3D Au/CNT-GF electrodes. (a) CEs of these three electrodes at a current of 1 mA cm-2 with a capacity of 1 mAh cm-2. (b) The rate performance of Cu, 3D CNT-GF and 3D Au/CNT-GF electrodes at different current densities with a capacity of 1 mAh cm-2. (c) Voltage-capacity curves of 3D CNT-GF and (d) 3D Au/CNT-GF electrodes at different current densities derived from (b). (e) Overpotentials of Cu, 3D CNT-GF and 3D Au/CNT-GF electrodes at different current densities. (f) EIS of 3D CNT-GF and 3D Au/CNT-GF electrodes before cycles and after the 30th cycle. Inset shows the equivalent circuit model used for EIS. (g) Voltage profiles of Cu, 3D CNT-GF and 3D Au/CNT-GF electrodes at 1 mA cm-2 with 1 mAh cm-2. Insert shows the short circuit curve of Cu electrode at 75 h. (h) Voltage profiles of 3D Au/CNT-GF anode at 5 mA cm-2 with 1 mAh cm-2.

Table 1. Interface resistance and charge transfer resistance of 3D CNT-GF and 3D Au/CNT-GF electrodes before cycles and after 30th cycles.

Sample	R_s (Ω)	R_ct (Ω)
3D CNT-GF before cycles	3.6	117.5
3D CNT-GF 30th	2.1	21.0
3D Au/CNT-GF before cycles	2.6	99.3
3D Au/CNT-GF 30th	1.7	9.3

Table 2. Comparison of the electrochemical performance of various carbon-based Na metal hosts.

Materials	Electrolyte	Overpotential	Electrochemical performance (current density (mA cm^-2), areal capacity (mAh cm^-2), time (h))	Refs.
DGCF	NaPF₆ in diglyme	20 mV@1 mA cm^-2	1, 1, 1200	[83]
Empty Cell			2, 1, 1200
Au/CF	NaCF₃SO₃ in diglyme	3 mV @0.5 mA cm^-2	2, 1, 1000	[55]
NCF	NaPF₆ in diglyme	6 mV@0.25 mA cm^-2	2, 2, 3500	[84]
Empty Cell		10 mV@1 mA cm^-2	4, 2, 950
Empty Cell		27 mV@4 mA cm^-2
OCF	0.01 M NaTFSI + 1.0 M NaCF₃SO₃ in diglyme.	9 mV@0.5 mA cm^-2	0.5, 1, 8000	[85]
Empty Cell		11.4 mV@1 mA cm^-2	1, 1, > 3000
Empty Cell		12.7 mV@2 mA cm^-2	2, 1, 2000
Empty Cell		15.7 mV@5 mA cm^-2
NG-NF	NaPF₆ in diglyme	28 mV@0.5 mA cm^-2	0.5, 1, 800	[46]
Empty Cell			1, 1, 400
3D Au/CNT-GF	NaPF₆ in diglyme	2.1 mV@0.5 mA cm^-2	1, 1, 2600	This work
Empty Cell		2.8 mV@1 mA cm^-2	5, 1, 300
Empty Cell		4.3 mV@2 mA cm^-2
Empty Cell		5.9 mV@4 mA cm^-2
Empty Cell		12.1 mV@5 mA cm^-2

Fig. 5. (a) Schematic diagram of a full SIB with Na@3D Au/CNT-GF anode and NVP@C cathode. (b) Galvanostatic discharging/charging curves of NVP@C cathode (red line) and Na@3D Au/CNT-GF anode (black line). (c) Galvanostatic discharging/charging curves of the Na@3D Au/CNT-GF||NVP@C full battery at 100 mA g-1. (d) Cycling performance of Na@3D Au/CNT-GF||NVP@C full cell at 100 mA g-1.

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