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Rationally designing electrolyte additives for highly improving cyclability of LiNi_(0.5)Mn_(1.5)O_(4)/Graphite cells

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Journal of Energy Chemistry 2024年第4期91卷 266-275页

作者： Zhiyong Xia Kuan Zhou Xiaoyan Lin Zhangyating Xie Qiurong Chen Xiaoqing Li Jie Cai Suli Li Hai Wang Mengqing Xu Weishan Li School of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina China Zhuhai CosMX Battery Co. Ltd.Zhuhai 519180GuangdongChina National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)and Key Lab.of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006GuangzhouChina

High voltage is necessary for high energy lithium-ion batteries but difficult to achieve because of the highly deteriorated cyclability of the batteries.A novel strategy is developed to extend cyclability of a high voltage lithium-ion battery,LiNi_(0.5)Mn_(1.5)O_(4)/Graphite(LNMO/Graphite)cell,which emphasizes a rational design of an electrolyte additive that can effectively construct protective interphases on anode and cathode and highly eliminate the effect of hydrogen fluoride(HF).5-Trifluoromethylpyridine-trime thyl lithium borate(LTFMP-TMB),is synthesized,featuring with multi-functionalities.Its anion TFMPTMB-tends to be enriched on cathode and can be preferentially oxidized yielding TMB and radical TFMP-.Both TMB and radical TFMP can combine HF and thus eliminate the detrimental effect of HF on cathode,while the TMB dragged on cathode thus takes a preferential oxidation and constructs a protective cathode interphase.On the other hand,LTFMP-TMB is preferentially reduced on anode and constructs a protective anode interphase.Consequently,a small amount of LTFMP-TMB(0.2%)in 1.0 M LiPF6in EC/DEC/EMC(3/2/5,wt%)results in a highly improved cyclability of LNMO/Graphite cell,with the capacity retention enhanced from 52%to 80%after 150 cycles at 0.5 C between 3.5 and 4.8 V.The as-developed strategy provides a model of designing electrolyte additives for improving cyclability of high voltage batteries.

关键词： Electrolyte additive Design and synthesis cyclability High voltage batteries Cathode and anode interphases

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Three-dimensional ordered hierarchically porous carbon materials for high performance Li-Se battery

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Journal of Energy Chemistry 2022年第5期31卷 624-636页

作者： Hongyan Li Wenda Dong Chao Li Tarek Barakat Minghui Sun Yingying Wang Liang Wu Lang Wang Lei Xia Zhi-Yi Hu Yu Li Bao-Lian Su Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium Namur Institute of Structured Matter(NISM) University of NamurB-5000 NamurBelgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074HubeiChina

Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.

关键词： 3D ordered hierarchically porous carbon(OHPC) Shuttle effect cyclability High rate capability The generalized Murray’s law Li-Se batteries

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Lithium-ion modified cellulose as a water-soluble binder for Li-O2 battery

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Frontiers in Energy 2022年第3期16卷 502-508页

作者： Chenyi Hu Aiming Wu Fengjuan Zhu Liuxuan Luo Fan Yang Guofeng Xia Guanghua Wei Shuiyun Shen Junliang Zhang Institute of Fuel Cells School of Mechanical EngineeringMOE Key Laboratory of Power and Machinery EngineeringShanghai Jiao Tong UniversityShanghai200240China SJTU-Paris Tech Elite Institute of Technology Shanghai Jiao Tong UniversityShanghai200240China

An environment-friendly,water-soluble,and cellulose based binder(lithium carboxymethyl cellulose,CMC-Li)was successfully synthesized by using Li+to replace Na+in the commercial sodium carboxymethyl cellulose(CMC-Na).Li-O2 batteries based on the CMC-Li binder present enhanced discharge specific capacities(11151 mAh/g at 100 mA/g)and a superior cycling stability(100 cycles at 200 mA/g)compared with those based on the CMC-Na binder.The enhanced performance may originate from the electrochemical stability of the CMC-Li binder and the ion-conductive nature of CMC-Li,which promotes the diffusion of Li+in the cathode and consequently retards the increase of charge transfer resistance of the cathode during cycling.The results show that the water-soluble CMC-Li binder can be a green substitute for poly(vinylidene fluoride)(PVDF)binder based on organic solvent in the lithium oxygen batteries(LOBs).

关键词： cellulose binder specific capacity cyclability lithium-oxygen batteries

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Silk fibroin-based biopolymer composite binders with gradient binding energy and strong adhesion force for high-performance micro-sized silicon anodes

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Journal of Energy Chemistry 2023年第5期80卷 442-451,I0010页

作者： Panpan Dong Xiahui Zhang Julio Zamora John McCloy Min-Kyu Song School of Mechanical and Materials Engineering Washington State UniversityPullmanWashington 99164United States

Micro-sized silicon anodes have shown much promise in large-scale industrial production of high-energy lithium batteries.However,large volume change(>300%)of silicon anodes causes severe particle pulverization and the formation of unstable solid electrolyte interphases during cycling,leading to rapid capacity decay and short cycle life of lithium-ion batteries.When addressing such issues,binder plays key roles in obtaining good structural integrity of silicon anodes.Herein,we report a biopolymer composite binder composed of rigid poly(acrylic acid)(PAA)and flexible silk fibroin(SF)tailored for micro-sized silicon anodes.The PAA/SF binder shows robust gradient binding energy via chemical interactions between carboxyl and amide groups,which can effectively accommodate large volume change of silicon.This PAA/SF binder also shows much stronger adhesion force and improved binding towards high-surface/defective carbon additives,resulting in better electrochemical stability and higher coulombic efficiency,than conventional PAA binder.As such,micro-sized silicon/carbon anodes fabricated with novel PAA/SF binder exhibit much better cyclability(up to 500 cycles at 0.5 C)and enhanced rate capability compared with conventional PAA-based anodes.This work provides new insights into the design of functional binders for high-capacity electrodes suffering from large volume change for the development of nextgeneration lithium batteries.

关键词： Micro-sized silicon Binder Silk fbroin Strong adhesion force Rate capability cyclability

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LiF引发选择性锂化提升硅碳负极可逆容量

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Science China Materials 2022年第9期65卷 2335-2342页

作者：孙金燃张舒张庆华辛云川董杉木刘海胜李杰东王超鲁承龙杨武海刘亭亭马君谷林崔光磊 Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

Si@SiO_(x)/C复合负极具有较高比容量,被认为是锂离子电池实际工业应用中最有前途的负极材料.然而,由于硅的严重体积形变,复合负极的循环稳定性依然面临巨大挑战.本工作通过释放负极冗余容量中高度可逆的锂储存能力,提高了复合负极的循... 详细信息

Si@SiO_(x)/C复合负极具有较高比容量,被认为是锂离子电池实际工业应用中最有前途的负极材料.然而,由于硅的严重体积形变,复合负极的循环稳定性依然面临巨大挑战.本工作通过释放负极冗余容量中高度可逆的锂储存能力,提高了复合负极的循环稳定性.基于LiF与不同活性材料之间的界面分离能差,我们针对复合负极提出了一种LiF引发的选择性锂化策略.LiF在Si@SiO_(x)上发生再沉积并富集,分离LiC_(x)和Li_(15)Si_(4)的形成电位,进而促进锂离子在石墨中的存储(未修饰前复合负极中石墨的容量未被充分利用).因此,在不牺牲比容量的前提下,全电池获得了更好的倍率性能和循环性能.超高面容量(NCA/S450,4.9 mA h cm^(-2))的全电池经300次循环后,容量保持率从66.1%显著提高到94.2%.选择性锂化策略在实际工业应用中更加可行,不需要改变现有的电池制造工艺.本研究为长循环寿命硅/石墨复合负极的开发开辟了新途径.

关键词： silicon-based composite anode cyclability selective lithiation LiF interface separation energy

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Tris(trimethylsilyl) borate as an electrolyte additive for high-voltage lithium-ion batteries using LiNi_(1/3)Mn_(1/3)Co_(1/3)O_2 cathode

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Journal of Energy Chemistry 2016年第4期25卷 659-666页

作者： Chunfeng Yan Ying Xu Jianrong Xia Cuiran Gong Kerong Chen Key Laboratory of Coal to Ethylene Glycol and Its Related Technology Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences Fujian Chuangxin Science and Develops Co. Ltd.

The influence of tris(trimethylsilyl) borate (TMSB) as an electrolyte additive on lithium ion cells have been studied using Li/LiCo1/3Ni1/3Mn1/3O2 cells at a higher voltage, 4.7 V versus Li/Li+. 1 wt% TMSB can dramatically reduce the capacity fading that occurs during cycling at room temperature (RT) and elevated temperature (60 degrees C). After 150 cycles at 1 C rate (1 C= 278 mAh/g), the capacity retention of Li/LiCo1/3Ni1/3Mn1/3O2 is up to near 72% in the electrolyte with TMSB added, while it is only about 35% in the baseline electrolyte. The electrochemical behaviors, the surface chemistry and structure of Li/LiCo1/3Ni1/3Mn1/3O2 cathode are characterized with charge/discharge test, linear sweep voltammetry (LSV), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), thermal gravimetric analyses (TGA), scanning electron microscope (SEM) and transmission electron microscopy (TEM). These analysis results reveal that the addition of TMSB is able to protectively modify the electrode CEI film in a manner that suppresses electrolyte decomposition and degradation of electrode surface structure, even though at both a higher voltage of 4.7 V and an elevated temperature of 60 degrees C. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Tris(trimethylsilyl) borate (TMSB) Electrolyte additive High voltage RT and 60 degrees C cyclability

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Boosting lithium batteries under harsh operating conditions by a resilient ionogel with liquid-like ionic conductivity

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Journal of Energy Chemistry 2021年第11期30卷 408-414,I0009页

作者： Le Yu Qing Liu Libin Wang Songtao Guo Qiaomei Hu Yaqian Li Xiwei Lan Zhifang Liu Xianluo Hu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazlwng University of Science and TechnologyWuhan 430074HubeiChina

New chemistries are being developed to increase the capacity and power of rechargeable batteries. However, the risk of safety issues increases when high-energy batteries using highly active materials encounter harsh operating conditions. Here we report on the synthesis of a unique ionogel electrolyte for abuse-tolerant lithium batteries. A hierarchically architected silica/polymer scaffold is designed and fabricated through a facile soft chemistry route, which is competent to confine ionic liquids with superior uptake ability (92.4 wt%). The monolithic ionogel exhibits high conductivity and thermal/mechanical stability, featuring high-temperature elastic modulus and dendrite-free lithium cycling. The Li/LiFePO_(4) pouch cells achieve outstanding cyclability at different temperatures up to 150 ℃, and can sustain cutting, crumpling, and even coupled thermal–mechanical abuses. Moreover, the solid-state lithium batteries with LiNi_(0.60)Co_(0.20)Mn_(0.20)O_(2), LiNi_(0.80)Co_(0.15)Al_(0.05)O_(2), and Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2) cathodes demonstrate excellent cycle performances at 60 ℃. These results indicate that the resilient and high-conductivity ionogel electrolyte is promising to realize high-performance lithium batteries with high energy density and safety.

关键词： Ionogel electrolytes Lithium batteries Safety Harsh operating conditions cyclability

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KOH activated carbon derived from biomass-banana fibers as an efficient negative electrode in high performance asymmetric supercapacitor

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Journal of Energy Chemistry 2017年第1期26卷 56-62页

作者： ChaitraK Vinny R T Sivaraman P Narendra Reddy Chunyan Hu Krishna Venkatesh Vivek C S Nagaraju N Kathyayini N Department of Nanobiosciences Centre for Emerging TechnologiesJain Global CampusJain UniversityJakkasandra postKanakapura TalukRamanagara DistrictBangalore Rural 562112 KarnatakaIndia Naval Materials Research Laboratory DRDOAmbernathThane 421506India Department of Chemistry St.Joseph’s College P.G.Centre.46Langford RoadShanthinagarBangaloreKarnataka 560027India Research Resource Centre Visveswaraya Technological UniversityBelagaviIndia College of Chemistry Chemical Engineering and BiotechnologyDonghua UniversityShanghai 201620China National Engineering Research Center for Dyeing and Finishing of Textiles Donghua UniversityShanghai 201620China

Here we demonstrate the fabrication, electrochemical performance and application of an asymmetric supercapacitor (AS) device constructed with ss-Ni(OH)(2)/MWCNTs as positive electrode and KOH activated honeycomb-like porous carbon (K-PC) derived from banana fibers as negative electrode. Initially, the electrochemical performance of hydrothermally synthesized ss-Ni(OH)(2)/MWCNTs nanocomposite and K-PC was studied in a three-electrode system using 1 M KOH. These materials exhibited a specific capacitance (Cs) of 1327 Fig and 324 F/g respectively at a scan rate of 10 mV/s. Further, the AS device i.e., ss-Ni(OH)(2)/MWCNTs// K-PC in 1 M KOH solution, demonstrated a Cs of 156 F/g at scan rate of 10 mV/s in a broad cell voltage of 0-2.2 V. The device demonstrated a good rate capability by maintaining a Cs of 59 F/g even at high current density (25 A/g). The device also offered high energy density of 63 Wh/kg with maximum power density of 5.2 kW/kg. The AS device exhibited excellent cycle life with 100% capacitance retention at 5000th cycle at a high current density of 25 A/g. Two AS devices connected in series were employed for powering a pair of LEDs of different colors and also a mini fan. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Asymmetric supercapacitor device Activated porous carbon High energy density cyclability Power source

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A Generalization of Implicit Ore-condition for Hamiltonicity of k-connected Graphs

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Acta Mathematicae Applicatae Sinica 2020年第3期36卷 620-626页

作者： Jun-qing CAI Lin WANG School of Management Qufu Normal UniversityRizhao 276826China

In 2005,Flandrin et al.proved that if G is a k-connected graph of order n and V(G)=X1∪X2∪···∪Xk such that d(x)+d(y)≥n for each pair of nonadjacent vertices x,y∈Xi and each i with i=1,2,···,k,then G is hamiltonian.In order to get more sufficient conditions for hamiltonicity of graphs,Zhu,Li and Deng proposed the definitions of two kinds of implicit degree of a vertex v,denoted by id1(v)and id2(v),respectively.In this paper,we are going to prove that if G is a k-connected graph of order n and V(G)=X1∪X2∪···∪Xk such that id2(x)+id2(y)≥n for each pair of nonadjacent vertices x,y∈Xi and each i with i=1,2,···,k,then G is hamiltonian.

关键词： implicit degree Hamiltonian cycle cyclability

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High-capacity Li-rich Mn-based Cathodes for Lithium-ion Batteries

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Chinese Journal of Structural Chemistry 2020年第1期39卷 20-25,1页

作者： YIN Zu-Wei LI Jun-Tao HUANG Ling PAN Feng SUN Shi-Gang College of Energy Xiamen UniversityXiamen 361005China State Key Lab of Physical Chemistry of Solid Surface College ofChemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Advanced Materials Peking UniversityShenzhen Graduate SchoolShenzhen 518055China

Layered Li-rich Mn-based oxides are promising cathode materials for Li-ion batteries due to their high capacity and high operation voltage.However,their commercial applications are hindered by irreversible capacity loss in the first charge-discharge process,voltage decay during cycling,inefficient cyclability and rate capability.Many attempts have been performed to solve such issues,including the mechanism study and strategies to improve the electrochemical performance.This article provides a brief review and future perspective on the main challenges of the high-capacity Li-rich Mn-based cathodes for Li-ion batteries.

关键词： Li-ion batteries Li-rich Mn-based cathodes the first charge-discharge process voltage decay cyclability rate capability

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