• Journal of the Korean Electrochemical Society
• /
• v.27 no.3
• /
• pp.97-104
• /
• 2024

The electrodes of commercialized lithium secondary batteries are manufactured through a wet coating process, and the drying process (DC) is a very important factor as to electrode production speed and process cost. In this study, silicon anodes were manufactured under high-temperature (180 ℃) and low-temperature (50 ℃) DC to investigate the quality and the electrochemical performance of Si-electrodes according to DC. High-temperature DC can quickly evaporate the solvent in the Si-electrode slurry, improving the electrode production rate. However, this also causes the electrode composite to peel off from the current collector. As a result, the Si-electrode's adhesion weakened, and the electrode coating's quality deteriorated. In addition, the Si-electrode manufactured under high-temperature was found to have a thicker composite material than the Si-electrode manufactured under low-temperature. Si-electrodes manufactured under high-temperature had higher sheet resistance and lower electrical conductivity than those manufactured under low-temperature. Consequently, the Si-electrode manufactured under low-temperature showed 152.5% superior cycle performance compared to the Si-electrode manufactured under high-temperature. (Discharge capacities of Si-electrodes manufactured under high-temperature and low-temperature DC were 844 and 1287 mAh g^-1, respectively, after 300 cycles). Establishing the DC of Si-electrodes can easily provide new perspectives to improve the quality and stability of Si-electrodes.

• Journal of the Korean Electrochemical Society
• /
• v.27 no.2
• /
• pp.73-79
• /
• 2024

As the use of fossil fuels has gradually increased, so has the emission of greenhouse gases such as carbon dioxide, leading to environmental problems. As a result, lithium-ion batteries (LiB) have emerged as the solution to this issue. To manufacture medium to large-sized lithium-ion batteries (LiB), it requires electrodes with high capacity and fast charging capabilities. Silicon (Si) is considered a next-generation anode with high-capacity properties, so, reduced graphene oxide (rGO) was compounded with Si@resorcinol-formaldehyde resin (RF) composite to prevent the volume expansion of Si. It was confirmed that the composite anode prepared exhibited improved capacity and enhanced stability.

• Korean Chemical Engineering Research
• /
• v.58 no.1
• /
• pp.142-149
• /
• 2020

In this study, the electrochemical performance of Graphite/Silicon/Pitch composites as anode material was investigated to improve the low theoretical capacity of artificial graphite. Spherical artificial graphite surface was coated with polyvinylpyrrolidone (PVP) amphiphiles material to synthesize Graphite/Silica material by silica islands growth. The Graphite/Silicon/Pitch composites were prepared by petroleum pitch coating and magnesiothermic reduction. The Graphite/Silicon/Pitch composite electrodes manufactured using poly(vinylidene fluoride) (PVDF), carboxymethyl cellulose (CMC) and polyacrylic acid (PAA) binders. The coin type half cell was assembled using various electrolytes and additives. The Graphite/Silicon/Pitch composites were analysed by X-ray diffraction (XRD), scanning electron microscope (SEM) and a thermogravimetric analyzer (TGA). The electrochemical characteristics of Graphite/Silicon/Pitch composite were investigated by constant current charge/discharge, rate performance, cyclic voltammetry and electrochemical impedance spectroscopy. The Graphite/Silicon/Pitch composites showed high cycle stability at a graphite/silica/pitch ratio (1:4:8 wt%). When the electrode is prepared using PAA binder, the high capacity and stability is obtained. The coin type half cell assembled using EC: DMC: EMC electrolyte showed high initial capacity (719 mAh/g) and excellent cycle stability. The rate performance has an capacity retention (77%) at 2 C/0.1 C and an capacity recovery (88%) at 0.1 C / 0.1 C when the vinylene carbonate (VC) was added.

• Applied Chemistry for Engineering
• /
• v.27 no.4
• /
• pp.444-448
• /
• 2016

Hollow silicon/carbon (H-Si/C) composites as anode materials for lithium ion batteries were investigated to overcome the large volume expansion. H-Si/C composites were prepared as follows; hollow $SiO_2\;(H-SiO_2)$ was prepared by adding $NaBH_4$ to $SiO_2$ synthesized using $st{\ddot{o}}ber$ method followed by magnesiothermic reduction and carbonization of phenolic resin. The H-Si/C composites were analyzed by XRD, SEM, BET and EDX. To improve the capacity and cycle performance, the electrochemical characteristics of H-Si/C composites synthesized with various $NaBH_4$ contents were investigated by charge/discharge, cycle, cyclic voltammetry and impedance tests. The coin cell using H-Si/C composite ($SiO_2:NaBH_4=1:1$ in weight) in the electrolyte of $LiPF_6$ dissolved in organic solvents (EC : DMC : EMC = 1 : 1 : 1 vol%) has better capacity (1459 mAh/g) than those of other composition coin cells. It is found that the coin cell ($SiO_2:NaBH_4=1:1$ in weight) has an excellent capacity retention from 2nd cycle to 40th cycle.

• Proceedings of the Korean Institute of Electrical and Electronic Material Engineers Conference
• /
• 2003.11a
• /
• pp.602-606
• /
• 2003

Silicon has been developed as an alternate anode material for lithium secondary batteries. A simple approach to improve the electrical contact of silicon powder has described. Carbon-coated and silver-coated silicon have been prepared by chemical vapor deposition and electroless plating respectively. Assembled cells, which consisted of surface modified silicon, lithium foil and $Li^+$ contained organic electrolyte, have been studied using electrochemical methods. Carbon-coated silicon was improved in the electrochemical performance such as reversibility and resistance compared to surface-unmodified silicon.

• Applied Chemistry for Engineering
• /
• v.26 no.6
• /
• pp.674-680
• /
• 2015

A solvent-soluble polyimide (PI) polymeric binder was synthesized by a two-step reaction for silicon (Si) anodes for lithium-ion batteries. Polyamic acid was first prepared through ring opening between two monomers, bicyclo[2,2,2]oct-7-ene-2,3,5,6-tetracarboxylic dianhydride (BCDA) and 4,4-oxydianiline (ODA), followed by condensation reaction. Using the synthesized PI polymeric binder (molecular weight = ~10,945), the coating slurry was then prepared and Si anode was fabricated. For the control system, Si anode based on polyvinylidene fluoride (PVDF, molecular weight = ~350,000) having the same constituent ratio was prepared. During precycling, PI polymeric binder revealed much improved discharge capacity ($2,167mAh\;g^{-1}$) compared to that of using PVDF polymeric binder ($1,740mAh\;g^{-1}$), while the Coulombic efficiency of two systems were similar. PI polymeric binder improved the cycle retention ability during cycles compared to that of using PVDF, which is attributed to an improved adhesion property inside Si anode diminishing the dimensional stress during Si volume changes. The adhesion property of each polymeric binder in Si anode was confirmed by surface and interfacial cutting analysis system (SAICAS) (Si anode based on PI polymeric binder = $0.217kN\;m^{-1}$ and Si anode based on PVDF polymeric binder = $0.185kN\;m^{-1}$).

• Journal of the Korean Electrochemical Society
• /
• v.13 no.2
• /
• pp.116-122
• /
• 2010

A $Cu_3Si$ film electrode is obtained by Si deposition on a Cu foil using DC magnetron sputtering, which is followed by annealing at $800^{\circ}C$ for 10 h. The Si component in $Cu_3Si$ is inactive for lithiation at ambient temperature. The linear sweep thermammetry (LSTA) and galvano-static charge/discharge cycling, however, consistently illustrate that $Cu_3Si$ becomes active for the conversion-type lithiation reaction at elevated temperatures (> $85^{\circ}C$). The $Cu_3Si$ electrode that is short-circuited with Li metal for one week is converted to a mixture of $Li_{21}Si_5$ and metallic Cu, implying that the Li-Si alloy phase generated at 0.0 V (vs. Li/$Li^+$) at the quasi-equilibrium condition is the most Li-rich $Li_{21}Si_5$. However, the lithiation is not extended to this phase in the constant-current charging (transient or dynamic condition). Upon de-lithiation, the metallic Cu and Si react to be restored back to $Cu_3Si$. The $Cu_3Si$ electrode shows a better cycle performance than an amorphous Si electrode at $120^{\circ}C$, which can be ascribed to the favorable roles provided by the Cu component in $Cu_3Si$. The inactive element (Cu) plays as a buffer against the volume change of Si component, which can minimize the electrode failure by suppressing the detachment of Si from the Cu substrate.

• Journal of the Korean Electrochemical Society
• /
• v.19 no.3
• /
• pp.87-94
• /
• 2016

In order to improve performances of submicrometer-sized Si negative electrode which shows larger volumetric change than nano-sized Si, composite binders are introduced by blending between poly(phenanthrenequinone) (PPQ) conductive polymer binder and poly(acrylic acid) (PAA) having good adhesion strength due to its carboxyl functional group. Blending between PPQ and PAA shows an effect that the adhesion strength of the Si electrode with the composite conductive binder is greatly improved after blending and this makes its better stable cycle performance. Blending ratios between PPQ and PAA in this work are 2:1, 1:1, 1:2 (by weight) and the best capacity retention at 50th cycle is observed in the electrode with the blending ratio 2:1 (named QA21). This is because that PPQ plays a role of conductive carbon among the Si particles or between Si particles and Cu current collector and PAA binds effectively the particles and the current collector. According to this synergetic effect, the internal resistance of the Si electrode with the blending ratio 2:1 is the smallest value. In addition, the Si electrode with PPQ-PAA composite binder shows the better stable cycle performance than the electrode with conventional super-P conductive carbon (20 wt.%).

• Journal of the Korean Electrochemical Society
• /
• v.16 no.2
• /
• pp.85-90
• /
• 2013

Graphite is a commercial anode material to have the specific capacity of 372 mAh/g and the true density of 2.2 g/ml. Many effort had been pouring to find out the better material than graphite. Good candidates are silicon, tin, etc. Zinc is also a plausible candidate to have the specific capacity of 412 mAh/g and the true density of 7.14 g/ml. In this study, the Zn based anode material including indium and nickel as minor additives was synthesised. In order to get the homogeneouly mixed Zn-In-Ni composite material, the sol-gel method was used. The anode prepared by Zn-In-Ni composite material has the $1^{st}$ specific capacity of 910 mAh/g. Through prolonged charge-discharge cycling, the specific capacities were reduced to 365 (at $31^{st}$ cycle) and 378 mAh/g (at $62^{th}$ cycle). The $1^{st}$ Ah efficiency was 45% and Ah efficiencies were exhibited at the prolonged cycle.

• Journal of the Korean Electrochemical Society
• /
• v.26 no.3
• /
• pp.35-41
• /
• 2023

The carbon-coated silicon monoxide (c-SiO_x), which is a negative electrode active material for lithium-ion batteries (LIBs), has a limited cycle performance due to severe volume changes during cycles, despite its high specific capacity. In particular, the significant volume change of the active material can deform the electrode structure and easily damage the electron transfer pathway. To improve performance and mitigate electrode damage caused by volume changes, we replaced parts of the carbon black conducting agent with carbon nanotubes (CNTs) having a linear shape. The content of the entire conductive material in the electrode was fixed at 10% by mass, and the relative content of CNTs ranged from 0% to 25% by mass to prepare electrodes and evaluate electrochemical performance. As the CNT content in the electrode increased, both cycle life and rate capability improved. Even a small amount of CNT can significantly improve the electrochemical performance of a c-SiO_x negative electrode with large volume changes. Furthermore, dispersing CNTs effectively can lead to achieving the equivalent performance with a reduced quantity of CNTs.