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1,3,5-Trifluorobenzene endorsed EC-free electrolyte for high-voltage and wide-temperature lithium-ion batteries

Journal of Energy Chemistry 2023年第10期85卷 49-57,I0003页

作者： Mingsheng Qin ziqi zeng Qiang Wu Xiaowei Liu Qijun Liu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina

Ethylene carbonate(EC)is susceptible to the aggressive chemistry of nickel-rich cathodes,making it undesirable for high-voltage lithium-ion batteries(LIBs).The arbitrary elimination of EC leads to better oxidative tolerance but always incurs interfacial degradation and electrolyte ***,an EC-free electrolyte is deliberately developed based on gradient solvation by pairing solvation-protection agent(1,3,5-trifluorobenzene,F_(3)B)with propylene carbonate(PC)/methyl ethyl carbonate(EMC)formulation.F_(3)B keeps out of inner coordination shell but decomposes preferentially to construct robust interphase,inhibiting solvent decomposition and electrode ***,the optimized electrolyte(1.1 M)with wide liquid range(-70–77℃)conveys decent interfacial compatibility and high-voltage stability(4.6 V for LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2),NCM622),qualifying reliable operation of practical NCM/graphite pouch cell(81.1%capacity retention over 600 cycles at 0.5 C).The solvation preservation and interface protection from F_(3)B blaze a new avenue for developing high-voltage electrolytes in next-generation LIBs.

关键词： Lithium-ion batteries Solvation structure High-voltage electrolyte Wide-temperature range Interfacial chemistry

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Challenges and strategies of formulating low-temperature electrolytes in lithium-ion batteries

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Interdisciplinary Materials 2023年第2期2卷 308-336页

作者： Mingsheng Qin ziqi zeng Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhanChina State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina

Lithium-ion batteries(LIBs)have monopolized energy storage markets in modern *** reliable operation of LIBs at cold condition(<0°C),nevertheless,is inevitably hampered by the sluggish kinetics and parasite reactions,which falls behind the increasing demands for portable electronics and electric *** electrolyte controls both Li+transport and interfacial reaction,dictating the low-temperature performance ***,the rational formulation of electrolytes is significant for realizing superior lowtemperature performance and broadening application niches of ***,we first discuss the kinetic limitations of low-temperature LIBs,highlighting the importance of electrolyte structure and interfacial ***,the advancements for formulating subzero-temperature electrolyte are summarized with in-depth discussions about electrolyte formulation,solvation structure,interfacial chemistry,and low-temperature ***,some opportunities for lithium metal batteries and the corresponding lowtemperature electrolyte are ***,the major challenges and future perspectives are outlined for low-temperature LIBs.

关键词： electrolyte lithium-ion batteries low temperatures solvation structures

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Dual-Functional Organotelluride Additive for Highly Efficient Sulfur Redox Kinetics and Lithium Regulation in Lithium–Sulfur Batteries

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Energy & Environmental Materials 2023年第3期6卷 126-133页

作者： Wei Zhang Fenfen Ma Qiang Wu ziqi zeng Wei Zhong Shijie Cheng Xin Chen Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China GuSu Laboratory of Materials SuzhouJiangsu 215123China State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

High energy density and low cost made lithium–sulfur(Li–S)batteries appealing for the next-generation energy storage ***,their commercial viability is seriously challenged by serious polysulfide shuttle effect,sluggish sulfur kinetics,and uncontrollable dendritic Li ***,a dual-functional electrolyte additive,diphenyl ditelluride(DPDTe)is reported for Li–S *** sulfur cathodes,DPDTe works as a redox mediator to accelerate redox kinetics of sulfur,in which Te radical-mediated catalytic cycle at the solid–liquid interface contributes significantly to the whole *** lithium anodes,DPDTe can react with lithium metal to form a smooth and stable organic–inorganic hybrid solid-electrolyte interphase(SEI),enabling homogeneous lithium deposition for suppressing dendrite ***,the Li–S battery with DPDTe exhibits remarkable cycling stability and superb rate capability,with a high capacity up to 1227.3 mAh g^(-1)and stable cycling over 300 ***,a Li–S pouch cell with DPDTe is evaluated as the proof of *** work demonstrates that organotelluride compounds can be used as functional electrolyte additives and offers new insights and opportunities for practical Li–S batteries.

关键词： electrolyte additive Li anode Li2 S deposition Li–S battery sulfur kinetics

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Anion-Regulated Weakly Solvating Electrolytes for High-Voltage Lithium Metal Batteries

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Energy & Environmental Materials 2023年第6期6卷 259-265页

作者： Zhipeng Jiang Jisheng Mo Chen Li Haiwen Li Qingan Zhang ziqi zeng Jia Xie Yongtao Li School of Materials Science and Engineering&Low-Carbon New Materials Research Center Anhui University of TechnologyMaanshan 243002China Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials of Ministry of Education Anhui University of TechnologyMaanshan 243002China State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China Hefei General Machinery Research Institute Hefei 230031China

Development of advanced high-voltage electrolytes is key to achieving high-energy-density lithium metal batteries(LMBs).Weakly solvating electrolytes(WSE)can produce unique anion-driven interphasial chemistry via altering the solvating power of the solvent,but it is difficult to dissolve the majority of Li salts and fail to cycle at a cut-off voltage above 4.5 ***,we present a new-type WSE that is regulated by the anion rather than the solvent,and the first realize stable cycling of dimethoxyethane(DME)at 4.6 V without the use of the“solvent-in-salt”*** relationships between the degree of dissociation of salts,the solvation structure of electrolytes,and the electrochemical performance of LMBs were systematically *** found that LiBF_(4),which has the lowest degree of dissociation,can construct an anion-rich inner solvation shell,resulting in anion-derived anode/cathode *** to such unusual solvation structure and interphasial chemistry,the Li-LiCoO_(2)full cell with LiBF_(4)-based WSE could deliver excellent rate performance(115 mAh g^(-1)at 10 C)and outstanding cycling stability even under practical conditions,including high loading(10.7 mg cm^(-2)),thin Li(50μm),and limited electrolyte(1.2μL mg^(-1)).

关键词： high-voltage LiCoO_(2) lithium metal batteries solvation structure weakly solvating electrolyte

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Fermentation characteristics and probiotic activity of a purified fraction of polysaccharides from Fuzhuan brick tea

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Food Science and Human Wellness 2022年第3期11卷 727-737页

作者： Guijie Chen ziqi zeng Minhao Xie Yujia Peng Wangting Zhou Weiqi Xu Yi Sun Xiaoxiong zeng Zhonghua Liu College of Food Science and Technology Nanjing Agricultural UniversityNanjing 210095China Collaborative Innovation Center for Modern Grain Circulation and Safety College of Food Science and EngineeringNanjing University of Finance and EconomicsNanjing 210023China Key Laboratory of Ministry of Education for Tea Science Hunan Agricultural UniversityChangsha 410128China National Research Center of Engineering Technology for Utilization of Botanical Functional Ingredients Changsha 410128China

Polysaccharides from Fuzhuan brick tea(FBTPS),one of most important bioactive components in tea,showed various health-promoting *** previous work demonstrated that the crude FBTPS(CFBTPS)could modulate the gut ***,which purified fraction in CFBTPS contributing to the modulation of gut microbiota remains ***,the fermentation characteristics and probiotic activity of a purified fraction(FBTPS-2-1)of CFBTPS were evaluated in this *** results showed that gut microbiota could utilize FBTPS-2-1 to produce short-chain fatty acids including acetic,propionic,n-butyric and n-valeric ***-2-1 could modulate the structure and metabolic pathways of gut ***-2-1 could increase the health-promoting gut microbiota such as Prevotellaceae and Bifidobacteriaceae,and decreased the harmful bacteria such as Enterobacteriaceae and *** results of metagenomics showed that Prevotella copri and Megamonas funiformis were the dominant bacteria after fermentation of ***,FBTPS-2-1 could regulate the biosynthesis and metabolism pathways of gut ***,the enrichment of food with FBTPS-2-1 is expected as a potential strategy for promoting human health due to modulation of gut microbiota.

关键词： Fuzhuan brick tea Polysaccharide Fermentation characteristics Gut microbiota

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A model cathode for mechanistic study of organosulfide electrochemistry in Li-organosulfide batteries

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Journal of Energy Chemistry 2022年第3期31卷 440-447,I0012页

作者： Wei Zhang Fenfen Ma Sibei Guo Xin Chen ziqi zeng Qiang Wu Shuping Li Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina GuSu Laboratory of Materials Suzhou 215123JiangsuChina Hefei National Laboratory for Physical Sciences at the Microscale School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026AnhuiChina State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

Organosulfides offer new opportunities for high performance lithium-sulfur(Li-S)batteries because of materials abundance,versatile structures and unique ***,their redox kinetics as well as cycling performance need to be further *** redox mediators is a highly effective strategy to address above ***,the underlying mechanism in this chemistry is so far insufficiently ***,phenyl disulfide(Ph S–SPh)and phenyl diselenide(Ph Se–Se Ph)are used as a model system for mechanistic understanding of organosulfide electrochemistry,particularly the rate *** the reaction thermodynamics and charge-discharge process reveals redox of both S–S and C–S bonds,as well as that the coupling between radical exchange and electrochemical redox is the key to enhance the sulfur *** study not only establishes a basic understanding of orgaonsulfide electrochemistry in Li-S batteries,but also points out a general strategy for enhancing the kinetics of sulfur electrodes in electrochemical devices.

关键词： Organosulfide Radical exchange Reaction kinetics Rate acceleration

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High-safety and high-voltage lithium metal batteries enabled by nonflammable diluted highly concentrated electrolyte

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Nano Research 2024年第4期17卷 2638-2645页

作者： Han Zhang ziqi zeng Shuping Wang Yuanke Wu Changhao Li Mengchuang Liu Xinlan Wang Shijie Cheng Jia Xie State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Grid Anhui Electric Power Research Institute Anhui Province Key Laboratory of Electric Fire and Safety Protection(State Grid Laboratory of Fire Protection for Transmission and Distribution Facilities)Hefei 230601China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074China

Lithium metal batteries(LMBs)show great promise for achieving energy densities over 400 Wh·kg^(-1).However,highly flammable organic electrolytes are a long-lasting problem that triggers safety hazards and hinders the commercial application of ***,a nonflammable diluted highly concentrated electrolyte(DHCE)with ethoxy(pentafluoro)cyclotriphosphazene(PFPN)as a diluent is developed to simultaneously achieve high safety and cycling stability of high-voltage *** optimal DHCE not only ensures reversible Li deposition/dissolution behavior with a superior average Coulombic efficiency(CE)over 99.1%on lithium metal anode(LMA),but also suppresses side reactions and stress crack on the LiCoO_(2)(LCO)under high cut-off *** newly developed DHCE exhibits high thermal stability,showing complete nonflammability and reduced heat generation between the electrolyte and delithiated LCO/cycled *** work offers an opportunity for rational designing nonflammable electrolytes toward high-voltage and safe LMBs.

关键词： lithium metal batteries thermal stability nonflammable electrolyte high-voltage phosphazene

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Loosely coordinating diluted highly concentrated electrolyte toward -60℃ Li metal batteries

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Journal of Energy Chemistry 2024年第3期90卷 380-387,I0009页

作者： Han Zhang ziqi zeng Qiang Wu Xinlan Wang Mingsheng Qin Sheng Lei Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

Lithium metal batteries(LMBs) promise energy density over 400 Wh kg^(-1).However,they suffer severe electrochemical performance deterioration at sub-zero *** failure behavior highly correlates to inferior lithium metal anode(LMA) compatibility and sluggish Li^(+) ***,we demonstrate that cyclopentylmethyl ether(CPME) based diluted high-concentration electrolyte(DHCE)enables-60℃ LMBs *** leveraging the loose coordination between Li^(+) and CPME,such developed electrolyte boosts the formation of ion clusters to derive anion-dominant interfacial chemistry for enhancing LMA compatibility and greatly accelerates Li^(+) desolvation *** resulting electrolyte demonstrates high Coulombic efficiencies(CE),providing over 99.5%,99.1%,98.5% and 95% at 25,-20,-40,and-60℃*** assembled Li-S battery exhibits remarkable cyclic stability in-20,and-40℃ at 0.2 C charging and 0.5 C *** at-60℃,Li-S cell with this designed electrolyte retains> 70% of the initial capacity over 170 ***,lithium metal coin cell and pouch cell with10 mg cm^(-2) high S cathode loading exhibit cycling stability at-20℃.This work offers an opportunity for rational designing electrolytes toward low temperature LMBs.

关键词： Lithium metal batteries -60℃operation Lithium metal anode compatibility Li^(+) desolvation kinetics

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“In-N-out” design enabling high-content triethyl phosphate-based non-flammable and high-conductivity electrolytes for lithium-ion batteries

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Science China Chemistry 2024年第2期67卷 724-731页

作者： Mengchuang Liu Fenfen Ma Zicheng Ge ziqi zeng Qiang Wu Hui Yan Yuanke Wu Sheng Lei Yanli Zhu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan430074China GuSu Laboratory of Materials Suzhou215123China Institute of Metal Research Chinese Academy of SciencesShenyang110000China State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China

Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended *** use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of ***,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content *** mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate *** a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.

关键词： lithium-ion batteries graphite anode high-phosphate-content electrolytes non-flammable electrolyte excellent ion conductivity standard concentration

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Enabling an intrinsically safe and high-energy-density 4.5 V-class Li-ion battery with nonflammable electrolyte

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InfoMat 2020年第5期2卷 984-992页

作者： ziqi zeng Xingwei Liu Xiaoyu Jiang Zhenjie Liu Zhangquan Peng Xiangming Feng Weihua Chen Dingguo Xia Xinping Ai Hanxi Yang Yuliang Cao Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry and Molecular SciencesWuhan UniversityWuhanChina State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchunJilinChina College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhouChina Key Lab of Theory and Technology for Advanced Batteries Materials College of EngineeringPeking UniversityBeijingChina

Developing nonflammable electrolyte with a wide electrochemical window has become an urgent demand for high-energy-density and high-safe lithium-ion batteries(LIBs).Herein,a fluorinated nonflammable phosphate electrolyte is developed to construct a safe 4.5 V-class LIB(Si-SiC-C/0.35Li2MnO3-0.65LiNi0.5Mn0.5O2).The proposed fluorinated phosphate electrolyte,0.8 M LiPF6/tris(2,2,2-trifluoroethyl)phosphate(TFEP)+5 vol%fluoroethylene carbonate(FEC)+5 vol%vinylene carbonate(VC),is not only completely nonflammable but also exhibits excellent oxidative/reductive stability on 0.35Li2MnO30.65LiNi0.5Mn0.5O2 cathode and Si-SiC-C *** in situ differential electrochemical mass spectrometry and X-ray photoelectron spectroscopy proved that TFEP-based electrolyte does not decompose into gases but forms a high-quality electrode-electrolyte interface on cathode surface at high working *** 4.5 V-class LIBs using 0.8 M LiPF6 TFEP-based nonflammable electrolyte shed some light on potential application for high-safe and low-cost larger-scale energy storage.

关键词： high energy density lithium-ion battery nonflammable electrolyte safety

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