Electrophoretic deposition of a supercapacitor electrode of activated carbon onto an indium-tin-oxide substrate using ethyl cellulose as a binder

doi:10.1016/j.jmst.2020.03.072

Abstract

Abstract:

A transparent energy storage device is an essential component for transparent electronics. The increasing demand for high-power devices stimulates the development of transparent supercapacitors with high power density. A transparent electrode for such supercapacitors can be assembled via the electrophoretic deposition of an active material powder with a binder onto a transparent substrate. The properties of the binder critically influence the electrochemical behavior and performance of the resulting electrode. Ethyl cellulose (EC) is known as an eco-friendly, transparent, flexible, and inexpensive material. Here, we fabricated an electrode film with EC binder via electrophoretic deposition on an indium tin oxide (ITO) substrate instead of using the conventional polytetrafluoroethylene (PTFE) binder. The assembled electrodes with EC and PTFE were compared to investigate the feasibility of EC as a binder from different perspectives, including homogeneity, wettability, electrochemical behavior, and mechanical stability. The EC enabled the formation of a homogeneous film composed of smaller particles and with a higher specific capacitance compared with films prepared with PTFE. The annealing improved the adhesion strength of the EC because of its glass transition; however, its hydrophobic nature limited utilization of the active material for charge storage. Subsequent electrochemical activation improved the wettability of the electrode, resulting in an increased capacitance of 60 F g^-1. Furthermore, even with the lower wettability of EC compared with that of PTFE, better rate performance was possible with the EC electrode. The increased mechanical stability after the annealing process ensured an excellent cycle life of 95 % capacitance retention for 15,000 cycles.

Key words: Electrophoretic deposition, Transparent electrode, Activated carbon, Ethyl cellulose, Indium tin oxide

Taeuk Kim, Seong-Hoon Yi, Sang-Eun Chun. Electrophoretic deposition of a supercapacitor electrode of activated carbon onto an indium-tin-oxide substrate using ethyl cellulose as a binder[J]. J. Mater. Sci. Technol., 2020, 58: 188-196.

Figures/Tables 11

Fig. 1. Differential scanning calorimetry (DSC) and thermomechanical analysis (TMA) graphs for EC and PTFE.

Fig. 2. SEM images and corresponding EDS mapping images of an electrophoretic-deposited activated carbon electrode with (a, b) EC binder and (c, d) PTFE binder.

Fig. 3. (a) Particle size distribution and (b) SEM photos of the as-received activated carbon (AC) and electrophoretic-deposited film with EC binder.

Fig. 4. Cyclic voltammograms before and after the electrochemical activation of both the pristine and annealed electrodes with (a) EC binder and (d) PTFE binder (scan rate: 5 mV s-1, electrolyte: 0.5 M K2SO4). Nyquist spectra were plotted for an electrode with (b) EC and (e) PTFE measured at the open-circuit potential in the frequency range from 0.1 to 1,000 kHz. The contact angle was measured on electrodes with (c) EC and (f) PTFE for 20 min after the electrodes were annealed.

Table 1 Specific capacitance of the samples with different binders (measured at 5 mV s-1).

	Ethyl cellulose (EC)		Polytetrafluoroethylene (PTFE)
	Pristine	Annealed	Pristine	Annealed
Initial cycle	47 ± 3 F g^-1	33 ± 4 F g^-1	23 ± 1 F g^-1	40 ± 2 F g^-1
After 50 cycles	50 ± 2 F g^-1	60 ± 5 F g^-1	23 ± 1 F g^-1	41 ± 2 F g^-1

Table 2 Comparison of the relevant previous researches.

Active material	Conductive material	Binder	Substrate	Specific capacitance	Deposition technique	Ref.
Activated carbon (YP-50)	acetylene black	EC	nickel foil	158 F g^-1(20 mV s^-1) full-cell	Electrophoretic deposition (EPD)	[60]
Carbon nanotube (CNT)	-	EC + terpineol	carbon cloth	74 F g^-1 (2 mV s^-1) full-cell	Screen printing+ Atmospheric pressure plasma jet (APPJ)	[61]
Activated carbon (YP-50 F)	-	PTFE	aluminum foil	107 F g^-1 (0.1 A g^-1) full-cell	Rolling method	[62]
Activated carbon	carbon nanotubes	PTFE	nickel foam	156 F g^-1 (20 mV s^-1) half-cell	Dropping method	[63]
Activated carbon (Norit SX Ultra)	-	PTFE + CMC	nickel foam	80 F g^-1(10 mA cm^-2) full-cell	Laminating	[64]
Activated carbon (Norit SX Plus)	-	PTFE	stainless steel mesh	102 F g^-1 (0.35 mA cm^-2) half-cell	Spreading	[65]
Activated carbon (BCP)	-	PTFE	nickel gauze	150 F g^-1 (100 mA g^-1) half-cell	Hydraulic press	[66]
Activated carbon (Norit carbon)	Acetylene black	EC	ITO	60 F g^-1(5 mV s^-1) half-cell	Electrophoretic deposition (EPD)	Current work

Fig. 5. Rate capability of the electrophoretic-deposited electrodes with EC binder (red) and PTFE binder (blue) before (dotted line) and after (solid line) the annealing treatment.

Fig. 6. Digital images of the tapes detached from the electrodes assembled with EC and PTFE binders.

Table 3 Detached carbon from electrophoretic-deposited electrodes prepared with different binders (EC and PTFE). The values in parentheses are indexed on the basis of the ASTM D3359 standard table.

Binder	Areal ratio of carbon on tape (%)
Binder	Pristine	Annealed
EC	29 % (2B)	9 % (3B)
PTFE	65 % (1B)	62 % (1B)

Fig. 7. Long-term cyclability measured on (a) an electrode with EC and PTFE binder in a half-cell experiment for 15,000 cycles (cyclic voltammetry at 50 mV s-1) and (b) a symmetrical full-cell with an EC electrode (galvanostatic cycling at 0.4 A gboth electrodes-1).

Table 4 Long-term cycling results of the specific capacitance for 15,000 cycles.

	EC	PTFE
Initial cycle	41 F g^-1	34 F g^-1
15,000^th cycle	39 F g^-1 (95 %)	29 F g^-1 (85 %)

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