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Lithiophilic Li-Si alloy-solid electrolyte interface enabled by high-concentration dual salt-reinforced quasi-solid-state electrolyte

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Journal of Energy Chemistry 2024年第8期95卷 216-230,I0005页

作者： Yuanxing Zhang Ling Zhang Zhiguang Zhao Yuxiang Zhang Jingwen Cui Chengcai Liu Daobin Mu Yuefeng Su Borong Wu Feng Wu School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Chongqing Innovation Center Beijing Institute of TechnologyChongqing 401120China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing 100081China

Solid polymer electrolytes(SPEs)are urgently required to achieve practical solid-state lithium metal batteries(LMBs)and lithium-ion batteries(LIBs),Herein,we proposed a mechanism for modulating interfacial conduction and anode interfaces in high-concentration SPEs by *** electrolyte exhibits superior ionic conductivity and remarkable interface compatibility with salt-rich clusters:(1)polymer-plastic crystal electrolyte(P-PCE,TPU-SN matrix)dissociates ion pairs to facilitate Li+transport in the electrolyte and regulates Li^(+)diffusion in the *** crosslinking structure of the matrix compensates for the loss of mechanical strength at high-salt concentrations;(2)dual-anion TFSI^(-)_(n)-DFBOP^(-)_(m)in the Li^(+)solvation sheath facilitates facile Li^(+)desolvation and formation of salt-rich clusters and is conducive to the formation of Li conductive segments of TPU-SN matrix;(3)theoretical calculations indicate that the decomposition products of LiDFBOP form sei with lower binding energy with LiF in the SN system,thereby enhancing the interfacial electrochemical redox kinetics of SPE and creating a solid interface sei layer rich in *** a result,the optimized electrolyte exhibits an excellent ionic conductivity of9.31×10^(-4)S cm^(-1)at 30℃and a broadened electrochemical stability up to 4.73 *** designed electrolyte effectively prevents the formation of Li dendrites in Li symmetric cells for over 6500 h at0.1 mA cm^(-2).The specific Li-Si alloy-solid state half-cell capacity shows 711.6 mAh g^(-1)after 60 cycles at 0.3 A g^(-1).Excellent rate performance and cycling stability are achieved for these solid-state batteries with Li-Si alloy anodes and NCM 811 *** 811‖Prelithiated silicon-based anode solid-state cell delivers a discharge capacity of 195.55 mAh g^(-1)and a capacity retention of 97.8%after 120 *** 811‖Li solid-state cell also delivers capacity retention of 84.2%after 450 cycles.

关键词： Prelithiation Li-Si alloy anode Solid-state electrolyte sei layer

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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-NH2 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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Regulating the inner Helmholtz plane structure at the electrolyte-electrode interface for highly reversible aqueous Zn batteries

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Journal of Energy Chemistry 2024年第8期95卷 57-67,I0002页

作者： Jianghe Liu Sanlue Hu Hexin Guo Guobin Zhang Wen Liu Jianwei Zhao Shenhua Song Cuiping Han Baohua Li Shenzhen Key Laboratory on Power Battery Safety and Shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055GuangdongChina Shenzhen Key Laboratory of Advanced Materials School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055GuangdongChina Shenzhen HUASUAN Technology Co. Ltd.Shenzhen 518055GuangdongChina

The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite *** address these challenges,an inner Helmholtz plane(IHP)regulation method is proposed by employing low-cost,non-toxic maltitol as the electrolyte *** preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane,and thus hinder the immediate contact between Zn metal and H_(2)***,strong interaction between maltitol and H_(2)O molecules can restrain the activity of H_(2)***,the"IHP adsorption effect"along with the low LUMO energy level of maltitol-CF_(3)SO_(3)^(-)can promote the in-situ formation of an organic-inorganic complex solid electrolyte interface(sei)*** a result,the hydrogen/oxygen evolution side reaction,corrosion,and dendrites issues are effectively suppressed,thereby leading to highly reversible and dendrite-free Zn plating/*** Zn‖I_(2)battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability,showing a capacity retention of 75%over 20000 charge-discharge cycles at a large current density of 5 A g^(-1).In addition,the capacity of the device has almost no obvious decay over20000 cycles even at-30℃.This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.

关键词： Inner Helmholtz plane Adsorption effect Dendrite suppression sei layer Zn||I_(2)battery

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Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

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Journal of Energy Chemistry 2024年第7期94卷 568-576页

作者： Guntae Lim Dong Guk Kang Hyeon Gyu Lee Yen Hai Thi Tran Kihun An Junghyun Choi Kwang Chul Roh Do Youb Kim Seung-Wan Song Department of Chemical Engineering&Applied Chemistry Chungnam National University Daejeon 34134Republic of Korea Energy Storage Materials Center Korea Institute of Ceramic Engineering&TechnologyJinju 52851Republic of Korea Advanced Energy Materials Research Center Korea Research Institute of Chemical TechnologyDaejeon 34114Republic of Korea

Incorporation of higher content Si anode material beyond 5 wt% to Li-ion batteries(LIBs)is challenging,owing to large volume change,swelling,and solid electrolyte interphase(sei)instability ***,a strategy of diacetoxydimethylsilane(DAMS)additive-directed sei stabilization is proposed for a stable operation of Si-0.33FeSi_(2)(named as Si-Fe)anode without graphite,which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate(FEC)additive and reduce a dependence on *** stable cycling performance of highly loaded(3.5 mA h cm^(-2))pure Si-Fe anode is achieved with 2 wt%DAMS combined with 9 wt%FEC additives under ambient pressure,yielding high capacity 1270 mA h g^(-1)at 0.5 C and significantly improved capacity retention of 81% after 100 cycles,whereas short circuit and rapid capacity fade occur with FEC only ***-directed robust sei layer dramatically suppresses swelling and particles crossover through separator,and therefore prevents short circuit,demonstrating a possible operation of pure Si or Sidominant anodes in the next-generation high-energy-density and safe LIBs.

关键词： High-energy Li-ion battery Pure Si-Fe anode without graphite Silane additive sei layer Suppressed swelling

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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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Implanting a preferential solid electrolyte interphase layer over anode electrode of lithium ion batteries for highly enhanced Li^+ diffusion properties

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Journal of Energy Chemistry 2020年第9期29卷 285-292,I0009页

作者： Ye Kyu Kim Yoongon Kim Jaejin Bae Hyunwoo Ahn Yuseong Noh Hyunsu Han Won Bae Kim Department of Chemical Engineering Pohang University of Science and Technology(POSTECH)Nam-gu 37673PohangSouth Korea

The lithium-ion batteries are recognized as the most promising energy storage system,but it still does not meet the power requirements of electric vehicle batteries owing to low volumetric energy density with the traditional graphite electrode *** this study,we report the development of a novel electrode system fabricated by implantation of a solid electrolyte interphase(sei)layer on the graphite *** sei-implanted graphite electrode is made using a lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)-based electrolyte and cycled with a lithium tetrafluoroborate LiBF4-based *** new electrode system shows significantly enhanced electrochemical properties owing to the rapid and efficient diffusion of Li ions through the sei layer between the electrolyte and *** graphite electrode with its pre-formed sei layer achieves a reversible capacity of 357 mAh g^-1 at 0.5 C after 50 cycles,which is significantly higher than that of commercial lithium-ion battery systems constructed with LiPF6(312mAh g^-1).The resulting unique electrode system could present a new avenue in sei research for highperformance lithium-ion batteries.

关键词： sei layer Graphite Implanting Li ion diffusion LiTFSI LiBF4 Artificial Mobility

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