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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 LMBs.Here,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 LMBs.The 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 voltage.The newly developed DHCE exhibits high thermal stability,showing complete nonflammability and reduced heat generation between the electrolyte and delithiated LCO/cycled LMA.This 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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Understanding the failure mechanism towards developing high-voltage single-crystal Ni-rich Co-free cathodes

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Green Energy & Environment 2024年第6期9卷 1045-1057页

作者： Jixue Shen Bao Zhang Changwang Hao Xiao Li Zhiming Xiao Xinyou He Xing Ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China Zhejiang Power New Energy Co. Ltd.Zhuji311899China Material Science and Chemistry Engineering College China University of GeosciencesWuhan430074China

Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.

关键词： Li/Ni antisite defect Dynamic characteristic high-voltage Single-crystal Ni-rich Co-free cathodes Lithium-ion batteries

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Cyclic-anion salt for high-voltage stable potassium-metal batteries

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National Science Review 2022年第10期9卷 177-187页

作者： Yanyao Hu Ling Fan Apparao M.Rao Weijian Yu Caixiang Zhuoma Yanhong Feng Zhihui Qin Jiang Zhou Bingan Lu School of Physics and Electronics Hunan University Department of Physics and Astronomy Clemson Nanomaterials Institute Clemson University School of Materials Science and Engineering Central South University

Electrolyte anions are critical for achieving high-voltage stable potassium-metal batteries(PMBs).However,the common anions cannot simultaneously prevent the formation of ’dead K’ and the corrosion of Al current collector,resulting in poor cycling stability.Here,we demonstrate cyclic anion of hexafluoropropane-1,3-disulfonimide-based electrolytes that can mitigate the ’dead K’ and remarkably enhance the high-voltage stability of PMBs.Particularly,even using low salt concentration(0.8 M) and additive-free carbonate-based electrolytes,the PMBs with a high-voltage polyanion cathode(4.4 V) also exhibit excellent cycling stability of 200 cycles with a good capacity retention of 83%.This noticeable electrochemical performance is due to the highly efficient passivation ability of the cyclic anions on both anode and cathode surfaces.This cyclic-anion-based electrolyte design strategy is also suitable for lithium and sodium-metal battery technologies.

关键词： cyclic anion low concentration additive-free electrolyte high-voltage potassium-metal batteries solid-electrolyte interface

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Lithium plating-free 1 Ah-level high-voltage lithium-ion pouch battery via ambi-functional pentaerythritol disulfate

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能源化学:英文版 2023年第8期83卷 229-238,I0007页

作者： Dung Tien Tuan Vu Jinsol Im Jae-Hee Kim Jisoo Han Gyeong Jun Chung Giang Thi Huong Nguyen Junhyeok Seo Minjae Kim Eui-Hyung Hwang Young-Gil Kwon Jae Wook Shin Kuk Young Cho Seung-Wan Song Department of Chemical Engineering&Applied Chemistry Chungnam National UniversityDaejeon 34134Republic of Korea Department of Materials Science&Chemical Engineering Hanyang UniversityAnsan 15588Republic of Korea Fine Chem Co.Ltd. Daejeon 34365Republic of Korea d CSIM Co.Ltd. Yesan 32400Republic of Korea Dongwha Electrolyte Nonsan 32925Republic of Korea

Elevating the charge cut-off voltage beyond traditional 4.2 V is a commonly accepted technology to increase the energy density of Li-ion batteries(LIBs) but the risk of Li-dendrites and fire hazard increases as well. The use of ambi-functional additive, which forms stable solid electrolyte interphase(SEI) simultaneously at both cathode and anode, is a key to enabling a dendrites-free and well-working high-voltage LIB. Herein, a novel ambi-functional additive, pentaerythritol disulfate(PEDS), at 1 wt% without any other additive is demonstrated. We show the feasibility and high impacts of PEDS in forming lithium sulfateincorporated robust SEI layers at NCM523 cathode and graphite anode in 1 Ah-level pouch cell under4.4 V, 25 °C and 0.1 C rate, which mitigates the high-voltage instability, metal-dissolution and cracks on NCM523 particles, and prevents Li-dendrites at graphite anode. Improved capacity retention of 83%after 300 cycles is thereby achieved, with respect to 69% with base electrolyte, offering a promising path toward the design of practical high-energy LIBs.

关键词： Lithium-ion pouch cell Lithium plating-free high-voltage Ambi-functional additive SEI layer

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Hybrid solid electrolyte interphases formed in conventional carbonate electrolyte enable high-voltage and ultra-stable magnesium metal batteries

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Journal of Energy Chemistry 2023年第3期78卷 315-324,I0009页

作者： Yong Xie Huawei Song Siyang Ye Fei Tian Junjie Xie Danni Lei Chengxin Wang State Key Laboratory of Optoelectronic Materials and Technologies School of Materials Science and EngineeringSun Yat-sen(Zhongshan)UniversityGuangzhou 510275GuangdongChina

Magnesium metal batteries are considered as viable alternatives of lithium-ion batteries for their low cost and high capacity of magnesium.Nevertheless,the practical application of magnesium metal batteries is extremely challenging due to a lack of suitable electrolyte that can stabilize magnesium metal anode and high-voltage cathode simultaneously.Herein,we found that in-situ formed lithium/magnesium hybrid electrolyte interphases in conventional LiPF6-containing carbonate-based electrolyte can not only prevent the production of passivation layer on the magnesium metal anode,but also inhibit the oxidation of the electrolyte under high voltage.The symmetric magnesium‖magnesium battery can achieve reversible stripping/plating for 1600 and 600 h at 0.02 and 0.1 mA cm^(-2),respectively.In addition,when coupled with a carbon fiber cathode,the magnesium metal battery exhibited a capacity retention rate of 96.3% for 1000 cycles at a current density of 500 mA g^(-1)and presented a working voltage of ~3.1 V.This research paves a new and promising path to the commercialization process of rechargeable magnesium metal batteries.

关键词： Magnesium metal batteries high-voltage Carbonate electrolyte

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Rationalizing Na-ion solvation structure by weakening carbonate solvent coordination ability for high-voltage sodium metal batteries

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Journal of Energy Chemistry 2023年第12期87卷 105-113,I0004页

作者： Yan Deng Shuai Feng Zhiwen Deng Ye Jia Xuemei Zhang Changhaoyue Xu Sicheng Miao Meng Yao Kaipeng Wu Yun Zhang Wenlong Cai College of Materials Science and Engineering Sichuan UniversityChengdu 610064SichuanChina College of Chemistry and Chemical Engineering Taishan UniversityTaian 271000ShandongChina Engineering Research Center of Alternative Energy Materials and Devices Sichuan UniversityChengdu 610064SichuanChina

Commercial carbonate-based electrolytes feature highly reactive activities with alkali metals,yielding low Coulombic efficiencies and poor cycle life in lithium metal batteries,which possess much higher chemical activity in the rising star sodium metal batteries.To be motivated,we have proposed that decreasing the solvent solvation ability in carbonate-based electrolytes stepwise could enable longterm stable cycling of high-voltage sodium metal batteries.As the solvation capacity reduces,more anions are enticed into the solvation sheath of Na^(+),resulting in the formation of the more desirable interphase layers on the surface of the anode and the cathode.The inorganic-dominated interphases allow highly efficient Na^(+)deposition/stripping processes with a lower rate of dead sodium generation,as well as maintain a stable structure of the high-voltage cathode material.Specifically,the assembled Na||Na_(3)V_(2)(PO_(4))_(2)F_(3)battery exhibits an accelerated ion diffusion kinetics and achieves a higher capacity retention of 85.9%with during the consecutive 200 cycles under the high voltage of 4.5 V.It is anticipated that the tactics we have proposed could be applicable in other secondary metal battery systems as well.

关键词： Electrolyte Solvation structure Interfacial chemistry Sodium metal anode high-voltage

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An in-situ generated composite solid-state electrolyte towards high-voltage lithium metal batteries

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Science China Chemistry 2022年第5期65卷 934-942页

作者： Qinglei Wang Tiantian Dong Qian Zhou Zili Cui Xuehui Shangguan Chenglong Lu Zhaolin Lv Kai Chen Lang Huang Huanrui Zhang Guanglei Cui Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266100China School of Materials Science and Engineering Linyi UniversityLinyi 276000China School of Materials Science and Engineering Ocean University of ChinaQingdao 266042China

The solid-state electrolyte(SSE) has promising applications in next-generation lithium(Li) metal batteries(LMBs) because of its significantly enhanced safety and more compatible interface characteristics than flammable traditional liquid electrolytes.However,only a few attempts have achieved high-performance high-voltage LMBs,which is attributed to the fact that both high ionic conductivity and good compatibility with electrodes can hardly be achieved simultaneously.Herein,a composite solid-state electrolyte(CSE) based on star-shaped siloxane-based polymer electrolyte coupled with Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)ceramic fillers is designed and prepared through a facile in-situ polymerization method.The obtained CSE exhibits high ionic conductivity(i.e.,1.68 × 10^(-4) S cm^(-1) at a temperature of 60 ℃),superior anodic stability,and high Li-ion transference number(i.e.,0.53) because of the multifunctional synergistic effect of the polymer electrolyte with LLZTO ceramic fillers.Moreover,the as-developed CSE shows excellent compatibility with Li anodes.As a result,the as-developed CSE enables the development of long-life 4.4-V-class solid-state LMBs with a Li CoO_(2) cathode,with 79.7% capacity retention and 99.74% average Coulombic efficiency after 500 cycles at a 0.5 C rate.Postmortem analysis of cycled batteries confirms that such superior battery performance can be mainly ascribed to the formation of a compatible electrode/electrolyte interface.Furthermore,excellent safety features can be observed in LiCoO_(2)/Li pouch batteries.This work provides an important guide for the rational design of SSEs for high-voltage LMBs.

关键词： composite solid-state electrolyte in-situ lithium metal batteries high-voltage

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Effect of high-voltage thermal breakdown on pore characteristics of coal

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International Journal of Mining Science and Technology 2017年第6期27卷 1051-1055页

作者： Zhu Chuanjie Lu Ximiao Gao Zishan Yan Fazhi Guo Chang Zhang Xiangliang State Key Laboratory of Coal Mine Disaster Dynamics and Control Chongqing University School of Safety Engineering China University of Mining and Technology

high-voltage thermal breakdown has great potential application in permeability enhancement of coal seam. The characteristics of the breakdown channel, coal element, porosity and microscopic coal petrography of coal under high-voltage electric load were experimentally studied. The coal interior left apparent tracks due to electric current burning with high temperature. The percentage of C, O, Al, Fe, and Si had slightly decreased, while the content of element N increased obviously. Low-pressure nitrogen gas adsorption(LP-N_2GA) and mercury intrusion analysis showed that coal porosity increased. The increases of micropores and mesopores are beneficial to promotion of the ability of gas storage, and the increase of macropores could enhance the gas seepage and migration. The results of scanning electron microscope(SEM) show that there are many exogenous fractures in coal, which is also beneficial to gas seepage and migration. The results lay a theoretical foundation for application of high-voltage thermal breakdown in coal mines.

关键词： high-voltage thermal breakdown Permeability enhancement Porosity Fracture Gas adsorption

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Aqueous high-voltage all 3D-printed micro-supercapacitors with ultrahigh areal capacitance and energy density

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Journal of Energy Chemistry 2021年第12期30卷 514-520,I0012页

作者： Yu Liu Shuanghao Zheng Jiaxin Ma Yuanyuan Zhu Jiemin Wang Xinliang Feng Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina b Center for Advancing Electronics Dresden&Department of Chemistry and Food Chemistry.Technische Universitat Dresden DresdenGermany University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Dalian 116023Liaoning.China

With the rapid development of integrated and miniaturized electronics,the planar energy storage devices with high capacitance and energy density are in enormous demand.Hence,the advanced manufacture and fast fabrication of microscale planar energy units are of great significance.Herein,we develop aqueous planar micro-supercapacitors(MSCs) with ultrahigh areal capacitance and energy density via an efficient all-3 D-printing strategy,which can directly extrude the active material ink and gel electrolyte onto the substrate to prepare electrochemical energy storage devices.Both the printed active carbon/exfoliated graphene(AC/EG) electrode ink and electrolyte gel are highly processable with outstanding conductivity(~97 S cm^(-1) of electrode;-34.8 mS cm^(-1) of electrolyte),thus benefiting the corresponding shaping and electrochemical performances.Furthermore,the 3 D-printed symmetric MSCs can be operated stably at a high voltage up to 2.0 V in water-in-salt gel electrolyte,displaying ultrahigh areal capacitance of2381 mF cm^(-2) and exceptional energy density of 331 μWh cm^(-2),superior to previous printed micro energy units.In addition,we can further tailor the integrated 3 D-printed MSCs in parallel and series with various voltage and current outputs,enabling metal-free interconnection.Therefore,our all-3 D-printed MSCs place a great potential in developing high-power micro-electronics fabrication and integration.

关键词： 3D printing Micro-supercapacitors high-voltage Water-in-salt Graphene

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Revealing the correlation between structure evolution and electrochemical performance of high-voltage lithium cobalt oxide

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Journal of Energy Chemistry 2021年第3期30卷 786-794页

作者： Jiajia Wan Jianping Zhu Yuxuan Xiang Guiming Zhong Xiangsi Liu Yixiao Li Kelvin H.L.Zhang Chaoyu Hong Jianming Zheng Kai Wang Yong Yang Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfaceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021FujianChina Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina Ningde Amperex Technology Ltd Ningde 352100FujianChina School of Energy Xiamen UniversityXiamen 361005FujianChina

Lithium cobalt oxide(LCO)is the dominating cathode materials for lithium-ion batteries(LIBs)deployed in consumer electronic devices for its superior volumetric energy density and electrochemical performances.The constantly increasing demands of higher energy density urge to develop high-voltage LCO via a variety of strategies.However,the corresponding modification mechanism,especially the influence of the long-and short-range structural transitions at high-voltage on electrochemical performance,is still not well understood and needs further exploration.Based on ss-NMR,in-situ X-ray diffraction,and electrochemical performance results,it is revealed that the H3 to H1-3 phase transition dictates the structural reversibility and stability of LCO,thereby determining the electrochemical performance.The introduction of La and Al ions could postpone the appearance of H1-3 phase and induce various types of local environments to alleviate the volume variation at the atomic level,leading to better reversibility of the H1-3 phase and smaller lattice strain,and significantly improved cycle performance.Such a comprehensive long-range,local,and electronic structure characterization enables an in-depth understanding of the structural evolution of LCO,providing a guiding principle for developing high-voltage LCO for high energy density LIBs.

关键词： Lithium cobalt oxide high-voltage In-situ XRD Solid-state NMR Structure change

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