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A hydrophilic poly(methyl vinyl ether-alt-maleic acid) polymer as a green, universal, and dual-functional binder for high-performance silicon anode and sulfur cathode

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Journal of Energy Chemistry 2021年第11期30卷 127-135,I0003页

作者： Hao Chen Zhenzhen Wu Zhong Su Luke Hencz Su Chen Cheng Yan Shanqing Zhang Centre for Clean Environment and Energy School of Environment and ScienceGold Coast CampusGriffith UniversityGold CoastQueensland 4222Australia School of Mechanical Medical&Process EngineeringQueensland University of Technology(QUT)BrisbaneQueensland 4000Australia

Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.

关键词： Dual-functional Aqueous binder silicon anode Sulfur cathode Lithium-ion batteries Lithium-sulfur batteries

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Monothetic and conductive network and mechanical stress releasing layer on micron-silicon anode enabling high-energy solid-state battery

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Rare Metals 2024年第3期43卷 1017-1029页

作者： Xiang Han Min Xu Lan-Hui Gu Chao-Fei Lan Min-Feng Chen Jun-Jie Lu Bi-Fu Sheng Peng Wang Song-Yan Chen Ji-Zhang Chen College of Materials Science and Engineering Co-Innovation Center of Efficient Processing and Utilization of Forestry ResourcesNanjing Forestry UniversityNanjing210037China Department of Physics Xiamen UniversityXiamen361005China Western Digital Corporation MilpitasCA95035USA

silicon has ultrahigh capacity,dendrite-free alloy lithiation mechanism and low cost and has been regarded as a promising anode candidate for solid-state *** to the low infiltration of solid-state electrolyte(SSE),not the unstable solid-electrolyte interphase(SEI),but the huge stress during lithiation-and delithiation-induced particle fracture and conductivity lost tend to be the main *** this study,starting with micron-Si,a novel monothetic carbon conductive framework and a MgO coating layer are designed,which serve as electron pathway across the whole electrode and stress releasing layer,*** addition,the in situ reaction between Si and SSE helps to form a LiF-rich and mechanically stable SEI *** a result,the mechanical stability and charge transfer kinetics of the uniquely designed Si anode are significantly ***,high initial Coulombic efficiency,high capacity and durable cycling stability can be achieved by applying the Si@MgO@C anode in *** example,high specific capacity of 3224.6 mAh·g^(-1)and long cycling durability of 200 cycles are *** work provides a new concept for designing alloy-type anode that combines surface coating on particle and electrode structure design.

关键词： Lithium-ion battery(LIB) Solid-state electrolyte(SSE) silicon anode Stress relief Coating

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Realizing high-performance all-solid-state batteries with sulfide solid electrolyte and silicon anode:A review

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Nano Research 2023年第3期16卷 3741-3765页

作者： Xinyang Wang Kuang He Siyuan Li Jiahui Zhang Yingying Lu State Key Laboratory of Chemical Engineering Institute of Pharmaceutical EngineeringCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou 311215China Zhejiang Yongtai Technology Co. Ltd.Taizhou 317000China

Sulfide solid electrolyte(SE)is one of the most promising technologies for all-solid-state batteries(ASSBs)because of its high ionic conductivity and ductile mechanical *** order to further improve the energy density of sulfide-based ASSBs and promote practical applications,silicon anodes with ultrahigh theoretical capacity(4,200 mAh·g^(−1))and rich resource abundance have broad commercial ***,significant challenges including bulk instability of sulfide SEs and poor utilization of silicon materials have severely impeded the ASSBs from becoming *** this review,we first introduce the critical bulk properties of sulfide SEs and the most recent improving strategies covering the ionic conductivity,air stability,electrochemical window,mechanical stability,thermostability and solvent ***,we introduce the main factors affecting the compatibility of silicon and sulfide SE,including the carbon’s effect,particle size of silicon,external pressure,silicon composite matrix and the depth of silicon’s ***,we discuss possible research directions in the *** hope that this review can provide a comprehensive picture of the role of nanoscale approaches in recent advances in ASSBs with sulfide and silicon,as well as a source of inspiration for future research.

关键词： all-solid-state battery sulfide solid electrolyte silicon anode nanoscale optimization

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Stress-dissipated conductive polymer binders for high-stability silicon anode in lithium-ion batteries

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Journal of Materiomics 2023年第2期9卷 378-386页

作者： Zhong Xu Xiang Chu Keli Wang Haitao Zhang Zhongqian He Yanting Xie Weiqing Yang Key Laboratory of Advanced Technologies of Materials(Ministry of Education) School of Material Science and EngineeringSouthwest Jiaotong UniversityChengdu610031China College of Physics Sichuan UniversityChengdu641500China State Key Laboratory of Traction Power Southwest Jiaotong UniversityChengdu610031China

silicon-based anodes with high theoretical capacity have intriguing potential applications for high energy density lithium-ion batteries(LIBs),while suffer from immense volumetric change and brittle solidstate electrolyte interface that causes collapse of ***,a stress-dissipated conductive polymer binder(polyaniline with citric acid,PC)is developed to enhance the mechanical electrochemical performance between Si nanoparticles(SiNPs)and *** from the stable triangle network node of citric acid and a considerable distributed of hydroxyl groups,the PC binder can effectively dissipate the stress from SiNPs,thus providing an excellent cyclic stability of Si *** experimental results and theoretical calculation demonstrate the enhanced adhesion between binders and SiNPs could bond the particles tightly to form a robust *** as-fabricated Si anode exhibits outstanding structural stability upon long-term cycles that exhibit a highly reversible capability of 1021 mA·h·g^(-1)over 500 cycles at a current density of 0.5 C(1 C¼4200mA·g^(-1)).Evidently,this stressdissipated binder design will provide a promising route to achieve long-life Si-based LIBs.

关键词： Conductive polymer silicon anode Binder Mechanical electrochemistry Lithium-ion batteries

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Low‐temperature synthesis of graphitic carbon‐coated silicon anode materials

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Carbon Energy 2019年第2期1卷 246-252页

作者： Zheng Yan Huile Jin Juchen Guo Department of Chemical and Environmental Engineering University of California‐RiversideRiversideCalifornia College of Chemistry and Materials Engineering Wenzhou UniversityWenzhouChina

We report the synthesis of a high‐performance graphitic carbon‐coated silicon(Si@GC)composite material for lithium‐ion batteries via a scalable production *** Si is produced from the magnesiothermic reduction of commercial silica(SiO2)precursor followed by low‐temperature graphitic carbon coating using glucose as the *** obtained Si@GC composite achieves an excellent reversible specific capacity of 1195 mAh g−1 and outstanding cycle *** thick Si@GC anode(3.4 mg cm^−2)in full cells with commercial lithium iron phosphate cathode delivers a remarkable performance of 800 mAh g^−1 specific capacity and 2.7 mAh cm^−2 areal capacity as well as 93.6%capacity retention after 200 cycles.

关键词： glucose graphitic carbon Li‐ion batteries silicon anode

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Correlation between the physical parameters and the electrochemical performance of a silicon anode in lithium-ion batteries

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Journal of Materiomics 2019年第2期5卷 164-175页

作者： Guobin Zhu Yan Wang Siming Yang Qunting Qu Honghe Zheng College of Energy&Collaborative Innovation Center of Suzhou Nano Science and Technology Soochow UniversitySuzhouJiangsu215006PR China

Lithium-ion battery anode used as silicon particles were obtained from different major suppliers,and they were characterized by different spectroscopic techniques and evaluated by electrochemical *** between the key physical parameters and electrochemical properties of the silicon particles were *** particle size,surface oxygen content,-OH content and physical appearance are found to strongly influence the electrochemical properties of the Si *** particle size of 100 nm has great promise for the practical application of Si nanoparticles in the lithium-ion battery *** inverse correlation between the oxygen content and the reversible capacity or first coulombic efficiency was ***-OH content by surface treatment contributes to enhanced cycling stability by the improved affinity between the Si particle and the water-soluble *** Si particles perform better compared to irregular particles,and agglomeration dramatically decreases the cycling stability of the Si *** the investigated Si particles,the sample that exhibited a reversible capacity of more than 2500 mAh g^(-1),a first coulombic efficiency of 89.26%and an excellent cycling stability,has great potential for use in the battery industry.

关键词： Lithium ionbatteries silicon anode Physical parameters Particle size Surface condition

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A review of the carbon coating of the silicon anode in highperformance lithium-ion batteries

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新型炭材料（中英文） 2024年第5期39卷 896-917页

作者： XU Ze-yu SHAO Hai-bo WANG Jian-ming Department of Chemistry Zhejiang UniversityHangzhou 310058China

In the development of rechargeable lithium ion batteries(LIBs),silicon anodes have attracted much attention because of their extremely high theoretical capacity,relatively low Li-insertion voltage and the availability of silicon ***,their large volume expansion and fragile solid electrolyte interface(SEI)film hinder their commercial *** solve these problems,Si has been combined with various carbon materials to increase their structural stability and improve their interface *** use of different carbon materials,such as amorphous carbon and graphite,as three-dimensional(3D)protective anode coatings that help buffer mechanical strain and isolate the electrolyte is detailed,and novel methods for applying the coatings are ***,carbon materials used as a protective layer still have some disadvantages,necessitating their *** developments have focused on modifying the protective carbon shells,and substitutes for the carbon have been suggested.

关键词： Lithium-ion batteries silicon anode 3D carbon coating Carbon

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A thick yet dense silicon anode with enhanced interface stability in lithium storage evidenced by in situ TEM observations

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Science Bulletin 2020年第18期65卷 1563-1569,M0004页

作者： Junwei Han Dai-Ming Tang Debin Kong Fanqi Chen Jing Xiao Ziyun Zhao Siyuan Pan Shichao Wu Quan-Hong Yang Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300350China International Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)Namiki 1-1Tsukubalbaraki 305-0044Japan CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Increasing the density and thickness of electrodes is required to maximize the volumetric energy density of lithium-ion batteries for practical ***,dense and thick electrodes,especially highmass-content(>50 wt%) silicon anodes,have poor mechanical stability due to the presence of a large number of unstable interfaces between the silicon and conducting components during *** we report a network of mechanically robust carbon cages produced by the capillary shrinkage of graphene hydrogels that can contain the silicon nanoparticles in the cages and stabilize the silicon/carbon *** situ transmission electron microscope characterizations including compression and tearing of the structure and lithiation-induced silicon expansion experiments,have provided insight into the excellent confinement and buffering ability of this interface-strengthened graphene-caged silicon nanoparticle anode ***,a dense and thick silicon anode with reduced thickness fluctuations has been shown to deliver both high volumetric(>1000 mAh cm^-3) and areal(>6 mAh cm^-2)capacities together with excellent cycling capability.

关键词： Lithium-ion battery silicon anode Interface stability In situ TEM Dense and thick electrodes

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Facilitating prelithiation of silicon carbon anode by localized high-concentration electrolyte for high-rate and long-cycle lithium storage

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Carbon Energy 2024年第6期6卷 216-233页

作者： Yuanxing Zhang Borong Wu Jiaying Bi Xinyu Zhang Daobin Mu Xin-Yu Zhang Ling Zhang Yao Xiao Feng Wu School of Materials Science and Engineering Beijing Institute of TechnologyBeijingChina Chongqing Innovation Center Beijing Institute of TechnologyChongqingChina College of New Energy Xi′an Shiyou UniversityXi′anChina Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhouChina Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjinChina

The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)***,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the *** thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical *** SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic ***,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G *** also leads to uniform decomposition and high stability of the SEI with abundant organic *** a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 *** 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.

关键词： localized high-concentration electrolytes prelithiation SEI layer silicon anode

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Lamellar sulfonated acid polymer-initiated in situ construction of robust LiF-rich SEI enabling superior charge transport for ultrastable and fast charging silicon anodes

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Journal of Energy Chemistry 2024年第11期98卷 134-143页

作者： Jungsoo Park Song Kyu Kang Junhyuk Ji Hwichan Ahn Gwan Hyeon Park Minho Kim Won Bae Kim Graduate Institute of Ferrous&Eco Materials Technology(GIFT) Pohang University of Science and Technology(POSTECH)77 Cheongam-roNam-guPohang-siGyeongsangbuk-do 37673Republic of Korea Department of Chemical Engineering Pohang University of Science and Technology(POSTECH)77 Cheongam-RoNam-guPohang-siGyeongsangbuk-do 37673Republic of Korea

The extreme volume expansion of the silicon(Si) anodes during repeated cycles seriously induces undesirable interfacial side reactions,forming an unstable solid electrolyte interphase(SEI) that degrades the electrode integrity and cycle stability in lithium-ion batteries,limiting their practical *** considerable efforts to stabilize the SEI through surface modification,challenges persist in the development of high-performance Si anodes that effectively regulate intrinsic SEI properties and simultaneously facilitate electron/ion ***,a highly conductive and organic electrolyte-compatible lamellar p-toluenesulfonic acid-doped polyaniline(pTAP) layer is proposed for constructing a robust artificial SEI on Si nanoparticles to achieve fast charging,lo ng-term cycle lifespan and high areal *** spatially uniform pTAP layer,formed through a facile direct-encapsulation approach assisted by enriched hydrogen bonding,contributes to the effective formation of in situ SEI with an even distribution of the LiF-rich phase in its interlamination ***,the integrated artificial SEI facilitates isotropic ion/electron transport,increased robustness,and effectively dissipates stress from volume ***,a notably high rate performance of 570 mA h g^(-1),even at a substantially high current density of 10 A g^(-1),is achieved with excellent cyclic stability by showing a superior capacity over 1430 mA h g^(-1) at 1 A g^(-1) after 250 cycles and a high areal capacity of ca.2 mA h cm^(-2) at 0.5 C in a full cell *** study demonstrates that the rational design of conductive polymers with SEI modulation for surface protection has great potential for use in high-energy-density Si anodes.

关键词： Lithium-ion battery silicon anode Conductive polymers Solid electrolyte interphase

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