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Tracking the phase transformation and microstructural evolution of Sn anode using operando synchrotron X-ray energy-dispersive diffraction and X-ray tomography

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Journal of Energy Chemistry 2023年第1期76卷 429-437,I0011页

作者： Kang Dong Fu Sun Andre Hilger Paul H.Kamm Markus Osenberg Francisco Garcia-Moreno ingo manke Institute of Applied Materials Helmholtz-Zentrum Berlin fur Materialien und EnergieHahn-Meitner-Platz 1Berlin 14109Germany Institute of Materials Science and Technology Technische Universitat BerlinHardenbergstraβe 36Berlin 10623Germany Qingdao Institute of BioEnergy and Bioprocess Technology Chinese Academy of Sciences189 Songling RoadQingdao 266101ShandongChina

Tin(Sn)holds great promise as an anode material for next-generation lithium(Li)ion batteries but suffers from massive volume change and poor cycling performance.To clarify the dynamic chemical and microstructural evolution of Sn anode during lithiation and delithiation,synchrotron X-ray energydispersive diffraction and X-ray tomography are simultaneously employed during Li/Sn cell operation.The intermediate Li-Sn alloy phases during de/lithiation are identified,and their dynamic phase transformation is unraveled which is further correlated with the volume variation of the Sn at particle-and electrode-level.Moreover,we find that the Sn particle expansion/shrinkage induced particle displacement is anisotropic:the displacement perpendicular to the electrode surface(z-axis)is more pronounced compared to the directions(x-and y-axis)along the electrode surface.This anisotropic particle displacement leads to an anisotropic volume variation at the electrode level and eventually generates a net electrode expansion towards the separator after cycling,which could be one of the root causes of mechanical detachment and delamination of electrodes during long-term operation.The unraveled chemical evolution of Li-Sn and deep insights into the microstructural evolution of Sn anode provided here could guide future design and engineering of Sn and other alloy anodes for high energy density Li-and Na-ion batteries.

关键词： Sn anode Li-Sn phase transformation X-ray tomography Operando X-ray diffraction Anisotropic displacement Digital volume correlation(DVC)

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High-Performance 3D Li-B-C-Al Alloy Anode and its Twofold Li Electrostripping and Plating Mechanism Revealed by Synchrotron X-Ray Tomography

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Energy & Environmental Materials 2023年第3期6卷 247-256页

作者： Fengcheng Tang Xia Zhang Markus Osenberg Chao Yang Haifeng Huang Andr Hilger Masyuki Uesugi Kentaro Uesug Akihisa Takeuchi ingo manke Fu Sun Libao Chen State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China Helmholtz-Zentrum Berlin für Materialien und Energie 14109 Berlin Germany College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Japan Synchrotron Radiation Research Institute(JASRI)/Spring-8 Sayo-gun Hyogo 679-5198Japan

The uncontrollable Li electrostripping and plating process that results in dendritic Li growth and huge volume change of Li anode limits the practicality of Li metal batteries(LMBs).To simultaneously address these issues,designing three-dimensional(3D),lithiophilic and mechanically robust electrodes seems to be one of the cost-effective strategies.Herein,a new 3D Li-B-C-Al alloy anode is designed and fabricated.The prepared 3D alloy anode exhibits not only superior lithiophilicity that facilitates uniform Li nucleation and growth but also sufficient mechanical stability that maintains its structural integrity.Superior performance of the prepared 3D alloy is demonstrated through comprehensive electrochemical tests.In addition,non-destructive and 3D synchrotron X-ray computed tomography(SX-CT)technique is employed to investigate the underlying working mechanisms of the prepared alloy anode.A unique twofold Li electrostripping and plating mechanism under different electrochemical cycling conditions is revealed.Lastly,improved performance of the full cells built with the 3D alloy anode and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode corroborate its potential application capability.Overall,the current work not only showcases the superiority of the 3D alloy as potential anode material for LMBs but also provides fundamental insights into its underlying working mechanisms that may further propel its research and development.

关键词： Li alloy Li metal anode Li metal battery Li-B-C-Al plating

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固态锂金属电池中不均匀离子通量介导的正负极耦合失效机制

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Science Bulletin 2023年第8期68卷 813-825,M0004页

作者：郑越张舒马君孙富 Markus Osenberg AndréHilger Henning Markötter Fabian Wilde ingo manke 胡中波崔光磊 Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijing 100049China Shandong Energy Institute Qingdao 266101China Institute of Applied Materials Helmholtz-Zentrum Berlin für Materialien und EnergieBerlin 14109Germany Department of Non-Destructive Testing Bundesanstalt für Materialforschung und-PrüfungBerlin 12205Germany Institute of Materials Physics Helmholtz-Zentrum HereonGeesthacht 21502Germany

本文通过联用无损三维同步辐射X射线断层扫描成像技术(SXCT)和其他非原位测试技术及有限元模拟,深入研究了LiNi0.8Co0.1Mn0.1O2|Li6PS5Cl|Li全固态电池的衰退机制.研究发现正极电化学-机械力学耦合失效诱导的反应异质性产生不均匀的锂... 详细信息

本文通过联用无损三维同步辐射X射线断层扫描成像技术(SXCT)和其他非原位测试技术及有限元模拟,深入研究了LiNi0.8Co0.1Mn0.1O2|Li6PS5Cl|Li全固态电池的衰退机制.研究发现正极电化学-机械力学耦合失效诱导的反应异质性产生不均匀的锂离子通量并传输到负极,进而导致不均匀的锂沉积、溶解行为及死锂的产生等.锂负极不均匀的电化学反应行为又反作用于正极并强化其反应异质性,形成一种正负极衰退互相促进的正强化机制.随着电池继续循环,正负极的不均匀反应加剧造成其结构破坏,同时正负极体积缩胀引起电解质巨大塑性变形,最终致使电池失效.对比实验表明采用LiZr_(2)(PO_(4))_(3)(LZP)对正极进行改性,不仅有效抑制了正极的电化学-机械力学耦合失效,而且显著提高了负极锂沉积-溶解均匀性和电解质的结构完整性.该研究首次提出了全固态金属锂电池正负极相互依赖、相互关联的失效机制,为提升全固态金属锂电池性能提供了新思路.

关键词： Current density distribution Lithium ion flux Solid-state lithium metal batteries Codependent failure mechanism Cathode deactivation

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Cautious interpretation of coulombic efficiency(CE) in lithium metal batteries

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Journal of Energy Chemistry 2021年第5期30卷 34-36页

作者： Fu Sun Dong Zhou Xiaogang Wang ingo manke Libao Chen Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina Ningbo Institute of Materials Technology&Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina Institute of Applied Materials Helmholtz-Zentrum Berlin fiir Materialien und EnergieHahn-Meitner-Platz 114109 BerlinCermany State Key Laboratory for Powder Metallurgy Central South UniversityChangsha 410083HunanChina

The soaring demand for electrical energy storage technologies stimulated by advanced portable devices, prospering electric vehicles, and large-scale grid storage applications have triggered explosive research on Li metal battery (LMB), which has been widely acknowledged as the most promising energy storage technology of the future that can break the energy-density bottleneck of the state-of-art lithium-ion battery (LIB) technology [1,2].

关键词： Coulombic efficiency Lithium metal anode Lithium metal battery Lithium ion battery

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Sodiophilic and conductive carbon cloth guides sodium dendrite-free Na metal electrodeposition

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Journal of Energy Chemistry 2021年第10期30卷 61-70,I0003页

作者： Haijun Liu Markus Osenberg Ling Ni André Hilger Libao Chen Dong Zhou Kang Dong Tobias Arlt Xiayin Yao Xiaogang Wang ingo manke Fu Sun Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences 266101 QingdaoShandongChina Institute of Applied Materials Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Hahn-Meitner-Platz 114109 BerlinGermany State Key Laboratory for Powder Metallurgy Central South University410083 ChangshaHunanChina Ningbo Institute of Materials Technology&Engineering Chinese Academy of Sciences 315201 NingboZhejiangChina

Sodium metal battery(SMB)technology is one of the most promising candidates for next-generation rechargeable energy storage systems due to its high theoretical capacity and economical costeffectiveness.Unfortunately,its practical implementation is hindered by several challenges including short life-span and fast capacity decay,which is closely related to the uncontrollable generation of the sodium dendrites.Herein,a nitrogen and oxygen co-doped three-dimensional carbon cloth with hollow tubular fiber units was constructed as the host material for Na plating(Na@CC)to tackle these challenges.The obtained composite electrode can effectively reduce the nucleation overpotential of Na,guide the homogeneous Na^(+)flux,increase the kinetics of Na electrodeposition,lower the effective current density and eventually suppress the formation of electrochemically inactive Na dendrites.As a result,batteries built with the Na@CC composites exhibited stable long-term cycling stability.To gain an in-depth and comprehensive understanding of such phenomena,non-destructive and three-dimensional synchrotron X-ray tomography was employed to investigate the cycled batteries.Moreover,the COMSOL Multiphysics simulation was further employed to reveal the Na electrodeposition mechanisms.The current work not only showcases the feasibility of currently proposed sodiophilic 3 D Na@CC composite electrode but also provides fundamental insights into the underlying working mechanisms that govern its outstanding electrochemical performance.

关键词： Na metal anode Dendrite-free electrode Sodiophilicity Synchrotron X-ray imaging Tomography

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Multitarget Thiol-Activated Tetrapyridyl Gold(Ⅲ)Complexes for Hypoxic Cancer Therapy

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CCS Chemistry 2024年第3期6卷 783-797页

作者： Xue-Quan Zhou Selda Abyar Imma Carbo-Bague Lan Wang Sebastian Türck Maxime ASiegler Uttara Basu ingo Ott Rongfang Liu Adriaan PIJzerman Sylvestre Bonnet Institute of Biopharmaceutical and Health Engineering Tsinghua Shenzhen International Graduate School(SIGS)Tsinghua UniversityShenzhen 518055 Leiden Institute of Chemistry Leiden University2333 CC Leiden Department of Chemistry Simon Fraser UniversityBurnabyBritish Columbia V5A 1S6 Institute of Medicinal and Pharmaceutical Chemistry Technische Universität Braunschweig38106 Braunschweig Department of Chemistry Johns Hopkins UniversityBaltimoreMaryland 21218 Division of Drug Discovery&Safety Leiden Academic Centre for Drug ResearchLeiden University2333 CC Leiden

Gold complexes have emerged as promising anticancer metallodrugs due to their efficient thioredoxin reductase(TrxR)inhibition,which disturbs the redox balance of cancer cells.However,in this model,the role of the ligand(s)coordinated to gold is often overlooked.In this work,we present a series of tetrapyridyl Au(Ⅲ)complexes that exhibit thiol-induced release of a Au(Ⅰ)ion and a tetrapyridyl ligand.The formation of a free Au(Ⅰ)center is responsible for the expected TrxR inhibition.Additionally,the released ligand,which was visible in cells due to its intense blue fluorescence,showed excellent binding properties to the hERG potassium channel.Moreover,these ligands ended up in the lysosomes,resulting in significant lysosome damage.Altogether,the Au(Ⅲ)complexes presented in this work showed broad-spectrum anticancer properties,both in hypoxic 2D monolayers and 3D tumor spheroids.We suggest that the interaction of the released Au(Ⅰ)center and the tetrapyridyl ligand with two different protein targets may combine into prodrugs that overcome hypoxia-induced drug deactivation.

关键词： anticancer Au(Ⅲ)complexes enzyme inhibtion potassium channel affinity lysosome damage cell imaging prodrug

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Gallai-Ramsey Number for the Union of Stars

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Acta Mathematica Sinica,English Series 2022年第8期38卷 1317-1332页

作者： Ya Ping MAO Zhao WANG Colton MAGNANT ingo SCHIERMEYER School of Mathematics and Statistics Qinghai Normal UniversityXining 810008P.R.China College of Science China Jiliang UniversityHangzhou 310018P.R.China Department of Mathematics Clayton State UniversityMorrowGA30260USA Technische Universit?t Bergakademie Freiberg Institut für Diskrete Mathematik und Algebra09596 FreibergGermany

Given a graph G and a positive integer k,define the Gallai–Ramsey number to be the minimum number of vertices n such that any k-edge coloring of Kn contains either a rainbow(all different colored)triangle or a monochromatic copy of G.In this paper,we obtain exact values of the Gallai–Ramsey numbers for the union of two stars in many cases and bounds in other cases.This work represents the first class of disconnected graphs to be considered as the desired monochromatic subgraph.

关键词： Ramsey theory Gallai-Ramsey number union of stars

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Tempering of exhausted T cells to comprehend their adaptive response for suitable clinical translation

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Cellular & Molecular Immunology 2023年第12期20卷 1401-1402页

作者： Amit Sharma ingo G.H.Schmidt-Wolf Department of Integrated Oncology Center for Integrated Oncology(CIO)BonnUniversity Hospital BonnBonnGermany

Although cancer immunotherapy has taken center stage,exhaustion of T cells is undeniably one of the major problems preventing it from being fully successful[1].Certainly,reversal of T-cell exhaustion or dysfunction is of great importance for developing new strategies and restoring immune function.Nevertheless,counterarguments about the adverse effect of reversing T-cell exhaustion(leading to overactivation of T cells and cytotoxicity)and even their irreversible properties have been quite common in scientific debates.With more to be discovered about the reasons for T-cell failure,a better understanding of the molecular factors/determinants[2,3]that shape/remodel“heterogeneous”dysfunctional T cells in cancer makes clear sense.Indeed,two recent publications in Nature immunology have described the intriguing perspective of T-cell exhaustion[4,5].Of interest,Vignali et al.focused on the hypoxia-driven CD39-dependent suppressor function of exhausted T cells,whereas Saadey et al.emphasized restoring the epigenetic balance of TGFβ1/BMP signaling in exhausted T cells to unlock responsiveness to immune checkpoint blockade therapy.

关键词： irreversible exhaustion publications

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Male mate choice in livebearing fishes： an overview

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Current Zoology 2018年第3期64卷 393-403页

作者： ingo SCHLUPP Department of Biology University of Oklahoma 730 Van Vleet Oval Norman OK 73019 USA

Although the majority of studies on mate choice focus on female mate choice, there is growing recognition of the role of male mate choice too. Male mate choice is tightly linked to 2 other phenomena: female competition for males and ornamentation in females. In the current article, I review the existing literature on this in a group of fishes, Poeciliidae. In this group, male mate choice appears to be based on differences in female quality, especially female size, which is a proxy for fecundity. Some males also have to choose between heterospecific and conspecific females in the unusual mating system of the Amazon molly. In this case, they typically show a preference for conspecific females. Whereas male mate choice is relatively well documented for this family, female ornamentation and female competition are not.

关键词：配偶选择钓鱼交配系统女性亚马逊竞争装饰男性

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Comparison of drug abuse in Germany and China

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Acta Pharmacologica Sinica 2007年第10期28卷 1505-1518页

作者： ingo Ilja MICHELS Office of the Federal Drug Commissioner Federal Ministry of HealthBerlin 10117Germany

Drug abuse has a long,but also different history in Germany and China.TheOpium War largely influenced the history of China in 19th century;however,China was once recognized as a drug-free nation for 3 decades from the 1950s tothe 1980s.Drug abuse has spread quickly since re-emerging as a national problemin China in the late 1980s.The number of registered drug abusers increased from70 000 in 1990 to more than 1 million by the end of 2005.In past decades,illicit drugtrafficking and production have swept most provinces in China,and drug abusehas caused many problems for both abusers and the community.One major drug-related problem is the spread of HIV,which has caused major social and economicdamage in China.Germany,the largest developed European country,also facesthe drug and addiction problem.Germany has about 150 000 heroin addicts,forwhom HIV/AIDS has become a serious threat since the mid 1980s.To control thedrug problem,the German Government adopted the"Action Plan on Drugs andAddiction"in 2003;the China Central Government approved a similar regulationin the antidrug campaign in 2005.Germany has experience in reducing drug-re-lated harm.The methadone maintenance treatment (MMT) program has run formore than 20 years and the public has become more tolerant of addicts.In 2003,China began the MMT program for controlling the spread of HIV/AIDS.It isnecessary for China to learn from developed countries to acquire success in itsantidrug campaign.In this review,we will go over the differences and similaritiesin drug abuse between Germany and China.The differences are related to history,population and economics,drug policy context,drug laws,HIV/hepatitis C virusinfection,the MMT program and so on.These 2 nations have drug abuse prob-lems with different histories and currently use different approaches to handleillicit drug marketing and use.The legal penalties for illicit drug offences reflectthe social differences of these 2 nations with respect to the seriousness of particu-lar types of crimes.The characteristics of th

关键词： drug abuse methadone maintenance treatment heroin HIV/AIDS harm reduction comparison Germany China

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