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Regulating interfacial stability of SiO_(x) anode with fluoride-abundant solid–electrolyte interphase by fluorine-functionalized additive

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Rare Metals 2024年第2期43卷 671-681页

作者： Subin Lee taeeun yim Advanced Batteries Laboratory Department of ChemistryIncheon National UniversityIncheon22012Republic of Korea Research Institute of Basic Sciences College of Natural ScienceIncheon National UniversityIncheon22012Republic of Korea

Silicon oxide(SiO_(x))has received remarkable attention as a next-generation battery material;however,the sudden decrease in the cycling retention constitutes a significant challenge in facilitating its ***(2,2,2-trifluoroethyl)phosphite(TTFP),which can control parasitic reactions such as the pulverization of SiO_(x)anode materials and electrolyte decomposition,has been proposed to improve the lifespan of the *** electrochemical reduction of TTFP results in solid-electrolyte interphase(SEI)layers that are mainly composed of LiF,which occur at a higher potential than the working potential of the SiO_(x)anode and carbonate-based *** electrolyte with TTFP exhibited a substantial improvement in cycling retention after 100 cycles,whereas the standard electrolyte showed acutely decreased *** thickness of the SiO_(x)anode with TTFP also changed only slightly without any considerable delamination spots,whereas the SiO_(x)anode without TTFP was prominently deformed by an enormous volume expansion with several internal *** cycled SiO_(x)anode with TTFP exhibited less increase in resistance after cycling than that in the absence of TTFP,in addition to fewer decomposition adducts in corresponding X-ray photoelectron spectroscopy(XPS)analyses between the cycled SiO_(x)*** results demonstrate that TTFP formed SEI layers at the SiO_(x)interface,which substantially reduced the pulverization of the SiO_(x)anode materials;in addition,electrolyte decomposition at the interface decreased,which led to improved cycling retention.

关键词： Lithium-ion batteries(LIBs) Silicon oxide anode Electrolyte Additive Solid-electrolyte interphases(SEI) Tris(2,2,2-trifluoroethyl)phosphite

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Calcium-and sulfate-functionalized artificial cathode–electrolyte interphases of Ni-rich cathode materials

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Rare Metals 2021年第10期40卷 2793-2801页

作者： Kwangeun Jung taeeun yim Department of Chemistry Incheon National UniversityIncheon 22012Republic of Korea

Ni-rich lithium nickel–cobalt-manganese oxides(NCM) are considered the most promising cathode materials for lithium-ion batteries(LIBs);however, relatively poor cycling performance is a bottleneck preventing their widespread use in energy systems. In this work, we propose the use of a dually functionalized surface modifier, calcium sulfate(CaSO_(4), CSO), in an efficient one step method to increase the cycling performance of Ni-rich NCM cathode materials. Thermal treatment of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode materials with a CSO precursor allows the formation of an artificial Ca-and SO_(x)-functionalized cathode–electrolyte interphase(CEI) layer on the surface of Ni-rich NCM cathode materials. The CEI layer then inhibits electrolyte decomposition at the interface between the Ni-rich NCM cathode and the electrolyte. Successful formation of the CSO-modified CEI layer is confirmed by scanning electron microscopy(SEM) and Fourier transform infrared(FTIR) spectroscopy analyses, and the process does not affect the bulk structure of the Ni-rich NCM cathode material. During cycling, the CSO-modified CEI layer remarkably decreases electrolyte decomposition upon cycling at both room temperature and 45 ℃, leading to a substantial increase in cycling retention of the cells. A cell cycled with a 0.1 CSO-modified(modified with 0.1% CSO)NCM811 cathode exhibits a specific capacity retention of90.0%, while the cell cycled with non-modified NCM811 cathode suffers from continuous fading of cycling retention(74.0%) after 100 cycles. SEM, electrochemical impedance spectroscopy(EIS), X-ray photoelectron spectroscopy(XPS), and inductively coupled plasma mass spectrometry(ICP-MS) results of the recovered electrodes demonstrate that undesired surface reactions such as electrolyte decomposition and metal dissolution are well controlled in the cell because of the artificial CSO-modified CEI layer present on the surface of Ni-rich NCM811 cathodes.

关键词： Lithium-ion battery Cathode Cathode–electrolyte interphase Calcium sulfate Electrochemical performance

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CO_(2)-adsorbent spongy electrode for non-aqueous Li–O_(2) batteries

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Journal of Energy Chemistry 2022年第2期31卷 646-653页

作者： Yiseul Yoo Giseung Lee Min-Gi Jeong Hun-Gi Jung Sunghee Shin Dongjin Byun taeeun yim Hee-Dae Lim Center for Energy Storage Research Korea Institute of Science and Technology(KIST)Hwarang-ro 14-gil 5Seongbuk-guSeoul 02792Republic of Korea Department of Materials Science and Engineering Korea University145 Anam-roSeongbuk-guSeoul 02841Republic of Korea Department of Chemistry Incheon National University119 Academy-roYeonsu-guIncheon 22012Republic of Korea Department of Chemical and Biological Engineering Korea UniversitySeoul 02841Republic of Korea

Regulation of the Li_(2)CO_(3) byproduct is the most critical challenge in the field of non-aqueous Li–O_(2) *** considerable efforts have been devoted to preventing Li_(2)CO_(3) formation,no approaches have suggested the ultimate solution of utilizing the clean Li_(2)O_(2) reaction instead of that of Li_(2)CO_(3).Even if extremely pure O_(2) is used in a Li–O_(2) cell,its complete elimination is impossible,eventually generating CO_(2) gas during *** this paper,we present the new concept of a CO_(2)-adsorbent spongy electrode(CASE),which is designed to trap the evolved CO_(2) using adsorption *** candidates composed of amine functional groups(–NH2)for capturing CO_(2) were screened,with quadrapurebenzylamine(QPBZA)exhibiting superior CO_(2)-adsorbing ability among the proposed ***,we fabricated the CASE by sandwiching QPBZA between porous carbon layers,which facilitated the transport of gaseous *** new electrode was demonstrated to effectively capture the evolved CO_(2) during charge,therefore altering the reaction pathways to the ideal *** is highly advantageous to mitigate the undesirable CO_(2) incorporation in the next discharge,resulting in improved *** novel concept of a CO_(2)-sponging electrode provides an alternative route to the realization of practically meaningful Li–O_(2) batteries.

关键词： Li-O_(2)battery Benzylamine CO_(2)adsorption Li_(2)CO_(3) Li_(2)O_(2) CO_(2)-sponging electrode

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Critical role of corrosion inhibitors modified by silyl ether functional groups on electrochemical performances of lithium manganese oxides

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Journal of Energy Chemistry 2020年第12期29卷 425-433页

作者： Min Ji Seong taeeun yim Department of Chemistry Incheon National UniversityYeonsu-gu 22012IncheonRepublic of Korea Research Institute of Basic Sciences College of Natural ScienceIncheon National UniversityYeonsu-gu 22012IncheonRepublic of Korea

Lithium manganese oxides(Li Mn2 O4, LMO) have attracted significant attention as important cathode materials for lithium-ion batteries(LIBs), which require fast charging based on their intrinsic electrochemical properties. However, these properties are limited by the rapid fading of cycling retention, particularly at high temperatures, because of the severe Mn corrosion triggered by the chemical reaction with fluoride(F-) species existing in the cell. To alleviate this issue, three types of silyl ether(Si–O)-functionalized task-specific additives are proposed, namely methoxytrimethylsilane, dimethoxydimethylsilane, and trimethoxymethylsilane. Ex-situ NMR analyses demonstrated that the Si-additives selectively scavenged the F-species as Si forms new chemical bonds with F via a nucleophilic substitution reaction due to the high binding affinity of Si with F-, thereby leading to a decrease in the F concentration in the cell. Furthermore, the addition of Si-additives in the electrolyte did not significantly affect the ionic conductivity or electrochemical stability of the electrolyte, indicating that these additives are compatible with conventional electrolytes. In addition, the cells cycled with Si-additives exhibited improved cycling retention at room temperature and 45 °C. Among these candidates, a combination of MTSi and the LMO cathode was found to be the most suitable choice in terms of cycling retention(71.0%), whereas the cell cycled with the standard electrolyte suffered from the fading of cycling retention triggered by Mn dissolution(64.4%). Additional ex-situ analyses of the cycled electrodes using SEM, TEM, EIS, XPS, and ICP-MS demonstrated that the use of Si-additives not only improved the surface stability of the LMO cathode but also that of the graphite anode, as the Si-additives prevent Mn corrosion. This inhibits the formation of cracks on the surface of the LMO cathode, facilitating the formation of a stable solid electrolyte interphase layer on the su

关键词： Lithium-ion batteries Lithium manganese oxide cathode Electrolyte additive Corrosion Silyl ether Fluoride scavenger

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Dually-functionalized Ni-rich layered oxides for high-capacity lithium-ion batteries

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Journal of Materials Science & Technology 2021年第27期86卷 70-76页

作者： Ji Won Kim Kwangeun Jung taeeun yim Department of Chemistry Incheon National University119 Academy-roYeonsu-guIncheon 22012Republic of Korea

Layered lithium nickel-cobalt-manganese oxides(NCM)have been highlighted as advanced cathode materials for lithium-ion batteries(LIBs);however,their low interfacial stability must be overcome to ensure stable cycling performance of the *** this work,we propose a one-step surface modification method that uses a task-specific precursor,N,N,N,N-tetraethylsulfamide(NTESA),to improve interfacial stability of Ni-rich NCM cathode *** unstable surface properties of Ni-rich NCM cathode material are improved by embedding an artificial cathode-electrolyte interphase(CEI)layer on the cathode surface by heat treatment of the Ni-rich NCM cathode material with an NTESA precursor at low *** material analyses indicate that this approach allows the formation of amine-and sulfone-functionalized CEI layers on the surface of Ni-rich NCM cathode material without changing the layered structure of the cathode ***-functionalized Ni-rich NCM cathode materials exhibit improved cycling retention after 100 cycles:for example,a cell cycled with a 3.0 NTESA-modified NCM811 cathode presents the highest retention ratio of 88.3%,whereas a cell cycled with a non-functionalized NCM811 cathode suffers from rapid fading of the cycling performance(68.4%).Our additional SEM,XPS,and EIS analyses indicate that electrolyte decomposition is suppressed during electrochemical cycling,thereby leading to smaller increases in the internal ***-MS analyses of the cycled anodes also indicate that the NTESA-based artificial CEI layer inhibits the dissolution of transition metal components from the Ni-rich NCM cathode materials,thereby contributing to an improved overall electrochemical performance of the cell.

关键词： Lithium-ion battery Cathode Cathode-electrolyte interphase N,N,N,N-Tetraethylsulfamide Electrochemical performance

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