• Journal of the Korean Electrochemical Society
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• v.15 no.3
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• pp.154-159
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• 2012

Structural volume change occurring on the Si-based anode battery materials during alloying/dealloying with lithium is noticed to be a major drawback responsible for a limited cycle life. Silicon monoxide has been reported to show relatively improved cycling performance compared to Si-containing materials for rechargeable lithium batteries, due to the structural buffering role of in-situ formed $Li_2O$ and lithium silicate during the reaction of silicon monoxide and lithium. Here we report improved cycling ability of interfacially stabilized Si-$SiO_2$-graphite composite anode using silane-based electrolyte additive for rechargeable lithium batteries, which includes low cost silicon dioxide for structural stabilization and graphite for enhanced conductivity.

• Korean Chemical Engineering Research
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• v.61 no.1
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• pp.32-38
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• 2023

In this study, the electrochemical properties of dopamine coated silicon/silicon carbide/carbon(Si/SiC/C) composite materials were investigated to improve cycle stability and rate performance of silicon-based anode active material for lithium-ion batteries. After synthesizing CTAB/SiO₂ using the Stöber method, the Si/SiC composites were prepared through the magnesium thermal reduction method with NaCl as heat absorbent. Then, carbon coated Si/SiC anode materials were synthesized through polymerization of dopamine. The physical properties of the prepared Si/SiC/C anode materials were analyzed by SEM, TEM, XRD and BET. Also the electrochemical performance were investigated by cycle stability, rate performance, cyclic voltammetry and EIS test of lithium-ion batteries in 1 M LiPF₆ (EC: DEC = 1:1 vol%) electrolyte. The prepared 1-Si/SiC showed a discharge capacity of 633 mAh/g and 1-Si/SiC/C had a discharge capacity of 877 mAh/g at 0.1 C after 100 cycles. Therefore, it was confirmed that cycle stability was improved through dopamine coating. In addition, the anode materials were obtain a high capacity of 576 mAh/g at 5 C and a capacity recovery of 99.9% at 0.1 C/0.1 C.

• Bulletin of the Korean Chemical Society
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• v.32 no.1
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• pp.145-148
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• 2011

The thermal behavior of lithiated Si anodes has been investigated using differential scanning calorimetry (DSC). In particular, the effect of Si particle size on the thermal stability of a fully lithiated Si electrode was investigated. For DSC measurements, a lithiated Si anode was heated in a hermetically sealed high-pressure pan with a polyvinylidene fluoride (PVDF) binder and a 1 M $LiPF_6$ solution in an ethylene carbonate (EC)-diethyl carbonate (DEC) mixture. The thermal evolution around $140^{\circ}C$ increases with lithiation and with decreasing particle size; this phenomenon is attributed to the thermal decomposition of the solid electrolyte interface (SEI) film. Exothermic peaks, following a broad peak at around $140^{\circ}C$, shift to a lower temperature with a decrease in particle size, indicating that the thermal stability of the lithiated Si electrode strongly depends on the Si particle size.

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.32 no.1
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• pp.70-77
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• 2019

$SiO_x$ nanoparticles were granulated, and their microstructures and effects on electrochemical behaviors were investigated. In spite of the promising electrochemical performance of $SiO_x$, nanoparticles have limitations such as high surface area, low density, and difficulty in handling during slurry processing. Granulation can be one solution. In this study, pelletizing and annealing were conducted to create particles with sizes of several decades of micron. Decrease in surface area directly influences the initial charge and discharge process when granules are applied as anode materials for Li-ion batteries. Lower surface area is key to decreasing the amount of irreversible phase-formation, such as $Li_2Si_2O_5$, $Li_2SiO_3$ and $Li_4SiO_4$, as well as forming the solid electrolyte interface. Additionally, aggregation of nanoparticles is required to obtain further enhancement of the electrochemical behavior due to restrictions that there be no $Li_4SiO_4$-related reaction during the first discharge process.

• Applied Chemistry for Engineering
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• v.25 no.6
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• pp.592-597
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• 2014

The graphite/$SiO_2$ composites as anode materials for lithium-ion batteries were prepared by sol-gel method to improve the graphite's electrochemical characteristics. The prepared graphite/$SiO_2$ composites were analysed by XRD, FE-SEM and EDX. The graphite surface modified by silicon dioxide showed several advantages to stabilize SEI layer. The electrochemical characteristics were investigated for lithium ion battery using graphite/$SiO_2$ as the working electrode and Li metal as the counter electrode. Electrochemical behaviors using organic electrolytes ($LiPF_6$, EC/DMC) were characterized by charge/discharge, cycle, cyclic voltammetry and impedance tests. The lithium ion battery using graphite/$SiO_2$ electrodes had better capacity than that of using graphite electrodes and was able to deliver a discharge capacity with 475 mAh/g at a rate of 0.1 C. Also, the capacity retention ratio of the modified graphite reaches 99% at a rate of 0.8 C.

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.19 no.7
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• pp.636-643
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• 2006

Si-C materials were synthesized by the heating the mixture of silicon and polyvinylidene fluoride (PVDF). The electrochemical properties of the Si-C materials as the high capacitive anode materials of lithium secondary batteries were evaluated by the galvanostatic charge-discharge test through 2032 type $Si-C{\mid}Li$ coin cells. Charge-discharge tests were performed at C/10 hour rate(C = 372 mAh/g). Initial discharge and charge capacities of $Si-C{\mid}Li$ cell using a Si-C material derived from PVDF(20wt.%) were found to be 1,830 and 526 mAh/g respectively. The initial discharge-charge characteristics of the developed Si-C electrode were analyzed by the electrochemical galvanostatic test adopting the capacity limited charge cut-off condition(GISOC). The range of reversible specific capacity IIE(intercalation efficiency at initial discharge-charge) and IICs(surface irreversible specific capacity) were 216 mAh/g, 68 % and 31 mAh/g, respectively.

• Journal of the Korean Chemical Society
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• v.60 no.5
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• pp.299-309
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• 2016

In this study, the physicochemical and electrochemical properties of carbon nanomaterials and synthesized nano-carbon/Si composites were studied. The nano-carbon/Si composites were ball-milled to a nano size and coated with pyrolytic carbon using Chemical Vapor Deposition (CVD). They were then finely mixed with respective nano-carbon materials. The physicochemical properties of samples were analyzed using Scanning Electron Microscopy (SEM), Energy Dispersive X-ray Spectroscopy (EDS), Raman spectroscopy, X-ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), and surface area analyzer. The electrochemical characteristics were investigated using the galvanostatic charge-discharge and cyclic voltammetry (CV) measurements. Three-electrode cells were fabricated using the carbon nanomaterials and nano-carbon/Si composites as anode materials and LiPF₆ and LiClO₄ as electrolytes of Li secondary batteries. Reversibility using LiClO₄ as an electrolyte was superior to that of LiPF₆ as the electrolyte. The initial discharge capacities of nano-carbon/Si composites were increased compared to the initial discharge capacities of nano-carbon materials.

• Korean Chemical Engineering Research
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• v.56 no.3
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• pp.320-326
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• 2018

In this study, Graphite/Silicon/Carbon (G/Si/C) composites were synthesized to improve the electrochemical properties of Graphite as an anode material of lithium ion battery. The prepared G/Si/C composites were analyzed by XRD, TGA and SEM. Also the electrochemical performances of G/Si/C composites as the anode were performed by constant current charge/discharge, rate performance, cyclic voltammetry and impedance tests in the electrolyte of $LiPF_6$ dissolved inorganic solvents (EC:DMC:EMC=1:1:1 vol%). Lithium ion battery using G/Si/C electrode showed better characteristics than graphite electrode. It was confirmed that as the silicon content increased, the capacity increased but the capacity retention ratio decreased. Also, it was shown that both the capacity and the rate performances were improved when using the Silicon (${\leq}25{\mu}m$). It is found that in the case of 10 wt% of Silicon (${\leq}25{\mu}m$), G/Si/C composites have the initial discharge capacity of 495 mAh/g, the capacity retention ratio of 89% and the retention rate capability of 80% in 2 C/0.1 C.

• Journal of Electrochemical Science and Technology
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• v.13 no.2
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• pp.269-278
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• 2022

Utilization of high-voltage electrolyte additive(s) at a small fraction is a cost-effective strategy for a good solid electrolyte interphase (SEI) formation and performance improvement of a lithium-rich layered oxide-based high-energy lithium-ion cell by avoiding the occurrence of metal-dissolution that is one of the failure modes. To mitigate metal-dissolution, we explored fluorinated dual-additives of fluoroethylene carbonate (FEC) and di(2,2,2-trifluoroethyl)carbonate (DFDEC) for building-up of a good SEI in a 4.7 V full-cell that consists of high-capacity silicon-graphite composite (15 wt% Si/C/CF/C-graphite) anode and Li_1.13Mn_0.463Ni_0.203Co_0.203O₂ (LMNC) cathode. The full-cell including optimum fractions of dual-additives shows increased capacity to 228 mAhg^-1 at 0.2C and improved performance from the one in the base electrolyte. Surface analysis results find that the SEI stabilization of LMNC cathode induced by dual-additives leads to a suppression of soluble Mn²⁺-O formation at cathode surface, mitigating metal-dissolution event and crack formation as well as structural degradation. The SEI and structure of Si/C/CF/C-graphite anode is also stabilized by the effects of dual-additives, contributing to performance improvement. The data give insight into a basic understanding of cathode-electrolyte and anode-electrolyte interfacial processes and cathode-anode interaction that are critical factors affecting full-cell performance.

• Journal of the Korean Electrochemical Society
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• v.20 no.4
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• pp.61-66
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• 2017

The cycle performance of Ti-Si alloy anode material for Li-ion batteries has been investigated as a function of loading level of electrode using a nodule type of substrate, in which the current collector of flat foil is also used for comparison. The Ti-Si alloy powders are prepared by mechanical alloying method. The electrodes with the nodule type of current collector exhibit enhanced cycling performance compared to those using the flat foil because the alloy particles are more strongly adhered to substrate and the stress caused by lithiation and delithiation reaction can be effectively relaxed by nodule-type morphology. It appears, however, that the cycle performance is critically dependent on the loading level of electrode, even when the nodule type of current collector is applied. With high loading level, cracks are initiated at surface of electrode due to a steep stress gradient through the electrode thickness during cycling, leading to capacity fading.