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Boosting fast interfacial Li^(+)transport in solid-state Li metal batteries via ultrathin Al buffer layer

Nano Research 2023年第5期16卷 6825-6832页

作者： Shengnan Zhang Qing Sun Guangmei Hou Jun Cheng Linna Dai Jianwei Li lijie ci Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education) Research Center for Carbon NanomaterialsSchool of Materials Science and EngineeringShandong UniversityJinan 250061China School of Light Industry and Engineering Qilu University of Technology(Shandong Academy of Sciences)Jinan 250353China State Key Lab of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China School of Science Hubei University of TechnologyWuhan 430068China University of Health and Rehabilitation Sciences Qingdao266071China

Na superionic conductor(NASICON)-type Li_(1.5)Al_(0.5)Ge_(0.5)P_(3)O_(12)(LAGP)solid state electrolytes(SSEs)have attracted significant interests thanks to the prominent ionic conductivity(>10^(–4)S·cm^(–1))at room temperature and superb stability in air.Unfortunately,its application has been hindered by the lithium dendrites and the intrinsic interfacial instability of LAGP towards metallic Li,etc.Herein,by magnetron sputtering(MS),an ultrathin Al film is deposited on the surface of the LAGP pellet(Al-LAGP).By in-situ alloying reaction,the spontaneously formed LiAl buffer layer inhibits the side reaction between LAGP SSEs and Li metal,induces the uniform distribution of interfacial electric field as well.Density functional theory(DFT)calculations demonstrate that the LiAl alloy surface promotes the diffusion of lithium atoms due to the lower energy barrier,thereby inhibiting the formation of lithium dendrites.Consequently,the Li/Al-LAGP-Al/Li symmetric cells show a low resistance of 210Ωand a durable lifespan over 1,200 h at a high current density of 0.1 mA·cm^(-2).Assembled all solid state lithium metal batteries(ASSLMBs)with LiFePO_(4)(LFP)cathode significantly improve cycle stability and rate performance,proving a promising stabilization strategy towards the NASIOCN type electrolyte/anode interface in solid state Li metal batteries.

关键词： Li_(1.5)Al_(0.5)Ge_(0.5)P_(3)O_(12) solid-state battery Li+transport interfacial modification Al buffer

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Facile construction of a multilayered interface for a durable lithium‐rich cathode

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Carbon Energy 2023年第9期5卷 74-87页

作者： Zhou Xu Yifei Yuan Qing Tang Xiangkun Nie Jianwei Li Qing Sun Naixuan ci Zhenjie Xi Guifang Han lijie ci Guanghui Min Key Laboratory for Liquid–Solid Structural Evolution&Processing of Materials(Ministry of Education) Research Center for Carbon NanomaterialsSchool of Materials Science and EngineeringShandong UniversityJinanChina College of Chemistry and Materials Engineering Wenzhou UniversityWenzhouChina School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)ShenzhenChina

Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue.The multilayer interface is visually observed using an atomic-resolution scanning transmission electron microscope and a high-resolution transmission electron microscope.Combined with the electrochemical characterization,the redox of lattice oxygen is suppressed during the initial charging.In situ X-ray diffraction and the high-resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial(de)lithiation,which further prevents lattice distortion during long cycling.As a result,the initial Coulombic efficiency of the modified LRMO is up to 87.31%,and the rate capacity and long-term cycle stability also improved considerably.In this work,a facile surface reconstruction strategy is used to suppress vigorous anionic redox,which is expected to stimulate material design in high-performance lithium ion batteries.

关键词： lattice oxygen release lithium‐rich manganese‐based oxide cathodes reconstructed multilayer interface spinel phase transition‐metal ion migration

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Safe and Stable Lithium Metal Batteries Enabled by an Amide-Based Electrolyte

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Nano-Micro Letters 2022年第3期14卷 120-133页

作者： Wanbao Wu Yiyang Bo Deping Li Yihong Liang Jichuan Zhang Miaomiao Cao Ruitian Guo Zhenye Zhu lijie ci Mingyu Li Jiaheng Zhang Sauvage Laboratory for Smart Materials Harbin Institute of Technology(Shenzhen)Shenzhen 518055People’s Republic of China Research Centre of Printed Flexible Electronics School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055People’s Republic of China School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055People’s Republic of China Department of Chemistry University of IdahoMoscowID 83844‑2343USA

The formation of lithium dendrites and the safety hazards arising from flammable liquid electrolytes have seriously hindered the development of high-energy-density lithium metal batteries.Herein,an emerging amide-based electrolyte is proposed,containing LiTFSI and butyrolactam in different molar ratios.1,1,2,2-Tetrafluoroethyl-2,2,3,3-tetrafluoropropylether and fluoroethylene carbonate are introduced into the amide-based electrolyte as counter solvent and additives.The well-designed amide-based electrolyte possesses nonflammability,high ionic conductivity,high thermal stability and electrochemical stability(>4.7 V).Besides,an inorganic/organic-rich solid electrolyte interphase with an abundance of LiF,Li3N and Li-N-C is in situ formed,leading to spherical lithium deposition.The formation mechanism and solvation chemistry of amide-based electrolyte are further inves-tigated by molecular dynamics simulations and density functional theory.When applied in Li metal batteries with LiFePO4 and LiMn2O4 cathode,the amide-based electrolyte can enable stable cycling performance at room temperature and 60℃.This study provides a new insight into the development of amide-based electrolytes for lithium metal batteries.

关键词： Amide-based electrolyte Nonflammable Inorganic/organic-rich solid electrolyte interphase Dendrite-free Lithium metal batteries

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Stable operation of polymer electrolyte-solid-state batteries via lonepair electron fillers

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Nano Research 2023年第11期16卷 12727-12737页

作者： Hongbin Liu Qing Sun Jun Cheng Hongqiang Zhang Xiao Xu Yuanyuan Li Zhen Zeng Yue Zhao Deping Li Jingyu Lu lijie ci State Key Laboratory of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China School of Science Harbin Institute of Technology(Shenzhen)Shenzhen 518055China Research Center for Carbon Nanomaterials Key Laboratory for Liquid–Solid Structural Evolution&Processing of Materials(Ministry of Education)School of Materials Science and EngineeringShandong UniversityJinan 250061China College of Materials and Chemistry China Jiliang UniversityHangzhou 310018China

Due to the increasing demand and wide applications of lithium-ion batteries,higher requirements have been placed on the energy density and safety.Polymer solid-state electrolytes have gained significant popularity due to their excellent interface compatibility and safety.However,their applications have been greatly restricted by the high crystallinity at room temperature,which hinders the transport of lithium ions.Herein,we utilize inorganic tubular fillers with abundant lone-pair atoms to reduce the crystallinity of the polyethylene oxide(PEO)solid-state electrolyte membrane and improve its ionic conductivity at room temperature,enabling stable operation of the battery.The tubular lone-pair-rich inorganic fillers play a key role in providing avenues for both internal and external charge transportation.The surface lone-pair electrons facilitate the dissociation and transport of lithium ions,while the internally tubular electron-rich layer attracts ions into the cavities,further enhancing the ion transport.After 100 cycles at room temperature,the lithium battery loaded with this solid-state electrolyte membrane delivers a specific capacity of 141.6 mAh·g−1,which is 51.3%higher compared to the membrane without the fillers.

关键词： nanotube filler polymer electrolyte ion transport room temperature(RT)operation

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Dissolution and recrystallization of perovskite induced by N-methyl-2-pyrrolidone in a closed steam annealing method

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Journal of Energy Chemistry 2019年第3期28卷 78-83页

作者： Lili Zhi Yanqing Li Xiaobing Cao Yahui Li Xian Cui lijie ci Jinquan Wei SDU & Rice Joint Center for Carbon Nanomaterials Key Laboratory for Liquid-Solid Structural Evolution & Processing of Materials (Ministry of Education)School of Materials Science and Engineering Shandong University Department of Physics Changji College State Key Laboratory of Crystal Materials Shandong University State Key Lab of New Ceramic and Fine Processing Education Ministry Key Laboratory for Advanced Materials Processing Technology School of Materials Science and Engineering Tsinghua University

High quality perovskite films with large columnar grains are greatly desired for efficient perovskite solar cells. Here, low volatility N-methyl-2-pyrrolidone(NMP) was added in MAI/IPA solution in a two-step spin-coating method, which promoted the conversion of lead iodide to perovskite. The perovskite films were annealed by a closed-steam annealing method to prolong the recrystallization process of perovskite films assisted by the residual NMP. It leaded to high quality CH_3NH_3PbI_3 perovskite films with large columnar grains due to its enhancement of the Oswald ripening. The large grain perovskite film leaded to efficient carrier transformation and injection, and low recombination. The photovoltaic performance of the perovskite solar cells was improved significantly.

关键词： Perovskite solar cell N-Methyl-2-pyrrolidone (NMP) Dissolution and recrystallization Closed-steam annealing Oswald ripening

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锂氧电池中基于自支撑Ag/δ-MnO_(2)纳米花正极的可逆LiOH化学

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Science China Materials 2022年第6期65卷 1431-1442页

作者： Linna Dai Qing Sun Yuqing Yao Huanhuan Guo Xiangkun Nie Jianwei Li Pengchao Si Jingyu Lu Deping Li lijie ci Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education) Research Center for Carbon NanomaterialsSchool of Materials Science and EngineeringShandong UniversityJinan 250061China State Key Laboratory of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China School of Science Harbin Institute of Technology(Shenzhen)Shenzhen 518055China

因放电产物对有机电解液具有高攻击性,使得锂-氧电池能量效率低和循环稳定性差的问题一直限制着其实际应用.与典型放电产物过氧化锂相比,氢氧化锂(LiOH)具有更好的化学和电化学稳定性.本文通过在碳纸上原位生长嵌有纳米银的花状二氧化... 详细信息

因放电产物对有机电解液具有高攻击性,使得锂-氧电池能量效率低和循环稳定性差的问题一直限制着其实际应用.与典型放电产物过氧化锂相比,氢氧化锂(LiOH)具有更好的化学和电化学稳定性.本文通过在碳纸上原位生长嵌有纳米银的花状二氧化锰作为锂-氧电池的正极(Ag/δ-MnO_(2)@CP),并证明了它能催化LiOH的可逆生成和分解.原位拉曼测试和理论计算表明Ag/δ-MnO_(2)催化放电中间体LiO2*与水分子解离的H+反应最终生成LiOH.以Ag/δ-MnO_(2)@CP为正极的锂-氧电池在潮湿氧气环境下表现出更高的比容量和放电平台.在电流密度为200 mA g^(−1)时,锂-氧电池的过电位仅为0.5 V,在500 mA h g^(−1)的限制比容量下可循环867圈.该工作为研究固相催化剂在锂-氧电池中的作用提供了新的思路,并将促进基于LiOH放电产物的锂-氧电池的实际应用.

关键词：有机电解液放电产物电化学稳定性能量效率氢氧化锂二氧化锰过电位自支撑

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Guest ions pre-intercalation strategy of manganese-oxides for supercapacitor and battery applications

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Journal of Energy Chemistry 2021年第9期30卷 480-493页

作者： Lina Chen Chongyang Hao Yamin Zhang Youri Wei Linna Dai Jun Cheng Hongqiang Zhang lijie ci State Key Lab of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055GuangdongChina Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061ShandongChina

Optimization of intrinsic structure of electrode materials plays decisive roles in promoting the development of energy storage systems to meet the fast-growing requirements in the market.Interlayer engineering has been proved to be an effective way to obtain adequate active sites,preferable ion diffusion channels and stable structure,thus enhance the performance of batteries.An in-depth understanding of the correlation among synthesis,structure and performance will significantly promote the development of excellent materials and energy storage devices.Therefore,in this review,recent advances in regards to cation preintercalation engineering in Mn-based electrode materials for rechargeable metal ion batteries are systematically summarized.Preintercalated guest cations can expand interlayer space to promote ion diffusion kinetics,serve as pillars to stabilize structure,control composition and valence to switch electrochemical behavior,thus improve the overall performance of secondary batteries.Moreover,the existing challenges and perspectives are provided for the interlayer engineering and its promotion to battery industry.

关键词： Interlayer engineering Electrode materials Energy storage devices

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Potassium pre-inserted K1.04Mn8O16 as cathode materials for aqueous Li-ion and Na-ion hybrid capacitors

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Journal of Energy Chemistry 2020年第7期29卷 53-61,I0002页

作者： Yamin Zhang Lina Chen Chongyang Hao Xiaowen Zheng Yixuan Guo Long Chen Kangrong Lai Yinghe Zhang lijie ci Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061ShandongChina School of Materials Science and Engineering Harbin Institute of TechnologyShenzhen 518055GuangdongChina Department of Physics Changji UniversityChangji 831100Xinjiang Uygur Autonomous RegionChina LEO group Co. Ltd.Shanghai 200000China

For the applications of aqueous Li-ion hybrid capacitors and Na-ion hybrid capacitors,potassium ions are pre-inserted into MnO2 tunnel structure,the as-prepared K1.04Mn8 O16 materials consist of nanoparticles and nanorods were prepared by facile high-temperature solid-state reaction.The as-prepared materials were well studied and they show outstanding electrochemical behavior.We assembled hybrid supercapacitors with commercial activated carbon(YEC-8 A)as anode and K1.04Mn8 O16 as cathode.It shows high energy and power densities.Li-ion capacitors reach a high energy density of 127.61 Wh kg-1 at the power density of 99.86 W kg-1 and Na-ion capacitor obtains 170.96 Wh kg-1 at 133.79 W kg-1.In addition,the hybrid supercapacitors demonstrate excellent cycling performance which maintain 97%capacitance retention for Li-ion capacitor and 85%for Na-ion capacitor after 10,000 cycles.

关键词： K1.04Mn8O16 Pre-inserted Li-ion hybrid capacitors Na-ion hybrid capacitors Electrochemical behavior

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Fast and stable K-ion storage enabled by synergistic interlayer and pore-structure engineering

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Nano Research 2021年第12期14卷 4502-4511页

作者： Deping Li Qing Sun Yamin Zhang Xinyue Dai Fengjun Ji Kaikai Li Qunhui Yuan Xingjun Liu lijie ci State Key Laboratory of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(shenzhen)Shenzhen518055China Research Center for Carbon Nanomaterials Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education)School of Materials Science and EngineeringShandong UniversityJinan250061China

Carbon-based material has been regarded as one of the most promising electrode materials for potassium-ion batteries(PIBs).However,the battery performance based on reported porous carbon electrodes is still unsatisfactory,while the in-depth K-ion storage mechanism remains relatively ambiguous.Herein,we propose a facile“in situ self-template bubbling”method for synthesizing interlayer-tuned hierarchically porous carbon with different metallic ions,which delivers superior K-ion storage performance,especially the high reversible capacity(360.6 mAh·g^(−1)@0.05 A·g^(−1)),excellent rate capability(158.6 mAh·g^(−1)@10.0 A·g^(−1))and ultralong high-rate cycling stability(82.8%capacity retention after 2,000 cycles at 5.0 A·g^(−1)).Theoretical simulation reveals the correlations between interlayer distance and K-ion diffusion kinetics.Experimentally,deliberately designed consecutive cyclic voltammetry(CV)measurements,ex situ Raman tests,galvanostatic intermittent titration technique(GITT)method decipher the origin of the excellent rate performance by disentangling the synergistic effect of interlayer and pore-structure engineering.Considering the facile preparation strategy,superior electrochemical performance and insightful mechanism investigations,this work may deepen the fundamental understandings of carbon-based PIBs and related energy storage devices like sodium-ion batteries,aluminum-ion batteries,electrochemical capacitors,and dual-ion batteries.

关键词： potassium-ion batteries synergistic interlayer and pore-structure engineering theoretical calculations carbonaceous electrode ex situ Raman technique

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Composite solid electrolyte of Na3PS4-PEO for all-solid-state SnS2/Na batteries with excellent interfacial compatibility between electrolyte and Na metal

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能源化学：英文版 2020年第2期29卷 73-78页

作者： Xiaoyan Xu Yuanyuan Li Jun Cheng Guangmei Hou Xiangkun Nie Qing Ai Linna Dai Jinkui Feng lijie ci SDU& Rice Joint Center for Carbon Nanomaterials Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials(Ministry of Education)School of Materials Science and EngineeringShandong UniversityJinan 250061ShandongChina

High ionic conductivity and superior interfacial stability of solid electrolytes at the electrodes are crucial factors for high-performance all-solid-state sodium batteries. Herein, a composite solid electrolyte Na3PS4-polyethylene oxide is synthesized by the solution-phase reaction method with an improved ionic conductivity up to 9.4 × 10-5 S/cm at room temperature. Moreover, polyethylene oxide polymer layer is wrapped homogeneously on the surface of Na3PS4 particles, which could effectively avoid the direct contact between Na3PS4 electrolyte and sodium metal, thus alleviate their side reactions. We demonstrate that all-solid-state battery SnS2/Na with the composite solid electrolyte Na3PS4-polyethylene oxide delivers an enhanced electrochemical performance with 230 m Ah/g after 40 cycles.

关键词： Composite solid electrolyte Na 3PS4 All-solid-state sodium battery SnS2

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