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Bonding VSe2 ultrafine nanocrystals on graphene toward advanced lithium-sulfur batterie

Nano Research 2020年第10期13卷 2673-2682页

作者： Wenzhi Tian Baojuan Xi Yu Gu Qiang Fu Zhenyu Feng Jinkui Feng Shenglin Xiong key laboratory of Clloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical Engineringand State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China key laboratory for Liquid Solid Structural Evolution&Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061China

Lithium–sulfur batteries have been attracting considerable research attention due to their high energy densities and low costs. However, one of their main challenges is the undesired shuttling of polysulfides, causing rapid capacity degradation. Herein, we report the first example of sulfiphilic VSe2 ultrafine nanocrystals immobilized on nitrogen-doped graphene to modify the battery separator for alleviating the shuttling problem. VSe2 nanocrystals provide numerous active sites for chemisorption of polysulfides as well as benefit the nucleation and growth of Li2S. Furthermore, the kinetic reactions are accelerated which is confirmed by higher exchange current density and higher lithium ion diffusion coefficient. And the first-principles calculations further show that the exposed sulfiphilic planes of VSe2 boost the redox of Li2S. When used as separators within the lithium sulfur batteries, the cell indicates greatly enhanced electrochemical performances with excellent long cycling stability and exceptional rate capability up to 8 C. Moreover, it delivers a higher areal capacity of 4.04 mAh·cm^−2 as well as superior cycling stability with sulfur areal loading up to 6.1 mg·cm^−2. The present strategy can encourage us in engineering novel multifunctional separators for energy-storage devices.

关键词： sulfiphilic VSe2 lithium–sulfur batteries nucleation and growth of Li2S polysulfide electrocatalysis shuttle effect

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Growth mechanisms for spherical Ni_(0.815)Co_(0.15)Al_(0.035)(OH)_(2) precursors prepared via the ammonia complexation precipitation method

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Journal of Energy Chemistry 2021年第2期30卷 379-386,I0013页

作者： Xi Yang Xuesong Huang Hancheng Shi Peng Dong Ding Wang Jianguo Duan Yingjie Zhang Nationl and Localfoint enginering laboratory for lithium-ion Batteres and Materials Ppreparation Techmology Key Laboratory of Advanced Batrery Materas of Yunnan ProvinceFaculty of Metalturgical and Energy EngineeringKunming University of Science and TechnologyKurnming 650093YunnanChina

The microstructures of precursors strongly affect the electrochemical performance of Ni-rich layerstructured cathode *** this study,the growth behaviour of Ni_(0.815)Co_(0.15)Al_(0.035)(OH)_2(NCA) prepared via the ammonia complexation precipitation method in a 50-L-volume continuously stirred tank reactor(CSTR) is studied in *** growth of Ni(OH)2-based hydroxide can be divided into a nucleation process,an agglomeration growth process,a process in which multiple growth mechanisms coexist,and an interface growth process over time,while the inner structure of the CSTR can be divided into a nucleation zone,a complex dissolution zone,a growth zone,and a maturation *** concentration of ammonium ions affects the growth habit of the primary crystal significantly due to its specific adsorption on the electronegative crystal *** the ammonia concentration is 2.0 mol L^(-1).The LiNi_(0.815)Co_(0.15)Al_(0.035)O_2 materials inherit the grain structure of the *** prepared from precursors with(1 0 1)preferential primary particles show a higher specific capacity and better rate performance than those that were prepared from(0 0 1) preferential primary particles,but the latter realize a better cycling performance than the former.

关键词： Lithium ion batteries Growth mechanism Spherical agglomerates Mixed hydroxide LiNi_(0.815)Co_(0.15)Al_(0.035)O_(2)

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Facile Synthesis of High Molecular Weight Polypeptides via Fast and Moisture Insensitive Polymerization of a-Amino Acid N-Carboxyanhydrides

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Chinese Journal of Polymer Science 2020年第10期38卷 1131-1140,I0007页

作者： Yue Ming Wu Wei-Wei Zhang Rui-Yi Zhou Qi Chen Chen-Yu Xie Heng-Xue Xiang Bin Sun Mei-Fang Zhu Run-Hui Liu State keylaboratory of Bioreactor enginering East China Uniersity of Science and TechnologyShanghai 200237China State key laboratory for Modification of Chemical Fibers and Polymer Materals College of Materias Science and EngineringDonghua UniversityShanghai 201620China key laboratory of Specally Functional Polymeric Materials and Related Technology(ECUST)Ministry of Education Key Laboratory for Ultrafine Materials of Ministry of EducationResearch Center for Biomedical Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

Polypeptides have been widely utilized in the fields of biomaterials and *** since N-carboxyanhydride(NCA)was reported by Hermann Leuchs in 1906,ring-opening polymerization of Ncas has been extensively used to prepare *** continuous innovations,it is still challenging to synthesize polypeptides in high molecular weight *** address this challenge,we developed KHMDS/NaHMDS initiated fast NCA polymerization that is also moisture tolerant,open-flask amenable and terminal *** NCA polymerization was able to proceed in most common solvents and meet the solubility requirement of variable NCA monomers and corresponding *** can initiate r benzy-L glutamate-N carboxyanhydride(BLG NCA)polymerization in a reaction rate 92 times faster than does hexylamine and 80 times faster than does *** NCA polymerization also demonstrated easy and fast synthesis of gram-scale long chain polypeptides in an open flask.

关键词： NCA polymerization Polypeptide Open vessel Fast polymerization High Mw

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Inter-and intramolecular adhesion mechanisms of mussel foot proteins

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Science China(Technological Sciences) 2020年第9期63卷 1675-1698页

作者： KAN YaJing WEI ZhiYong TAN QiYan CHEN YunFei Jiangsu key laboratory for Design and Manugacture of Micro-Nano Biomedical Iastruments and School of Mchanical Enginering.Southeast UniversityNanjing 211189China School of Mechanical Engineering Nanjing Institute of TechnologyNanjing 211167China

Mussel foot proteins(Mfps) secreted in the byssal plaque of marine mussels are widely researched for their relevance to mussel adhesion in water. As the abundant residue in the amino acid sequences of major adhesive proteins, 3,4-dihydroxyphenylalanine(Dopa) or its catecholic moiety plays a key role in both Mfp binding to surface and cohesive cross-linking of Mfps in byssal plaques. The binding performance of an Mfp significantly depends on the content and redox state of Dopa, whereas the types of interaction vary in line with different surface chemistries and p H conditions. Thorough understanding of mussel adhesion from a molecular perspective is crucial to promote the application of synthetic mussel-bionic adhesives. This article presents a brief review of the research progress on the adhesion mechanisms of Mfps, which further emphasizes the contributions of Dopamediated interactions and considers other amino acids and factors. The involved inter-and intramolecular interactions are responsible for not only the diverse adhesion capacities of an adhesive byssal plaque as mussel's adhesion precursor but also the formation and properties of the plaque structure.

关键词： mussel foot protein adhesion mechanism Dopa catechol surface forces apparatus

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Molecular-scale controllable conversion of biopolymers into hard carbons towards lithium and sodium ion batteries: A review

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Journal of Energy Chemistry 2022年第9期31卷 554-569,I0016页

作者： Li-Jing Xie Cheng Tang Ming-Xin Song Xiao-Qian Guo Xiao-Ming Li Jing-Xue Li Chong Yan Qing-Qiang Kong Guo-Hua Sun Qiang Zhang Fang-Yuan Su Cheng-Meng Chen cas key laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina University of Chinese Academy of Sciences Beijing 100049China Bejing keylaboratory of Green Chemical Reaction Engineering and Technology.Department of Chemical Engineering.Tsinghua University Bejing 100084China School o Chemical enginering and Advanced Materials The Universityof Adelaide.AdelaideSA 5005Ausralia Center of Biomass enginering/Cllge of Agronomy and Biotechnology China Agriultural UniversiyBeijing 100193China

Hard carbons are widely investigated as potential anodes for lithium and sodium ion batteries owing to their internally well-tailored textures(closed pores and defects) and large microcrystalline interlayer spacing. The renewable biomass is a green and economically attractive carbon source to produce hard carbons. However, the chemical and structural complexity of biomass has plagued the understanding of evolution mechanism from organic precursors to hard carbons and the structure-property *** makes it difficult to finely tune the microstructure of biomass-derived hard carbons, thus greatly restricting their high-performance applications. Most recently, the optimal utilization and controllable conversion of biomass-derived biopolymers(such as starch, cellulose and lignin) at the molecular level have become a burgeoning area of research to develop hard carbons for advanced *** the principal source of carbonaceous materials is from biomass pyrolysis, we firstly overview the chemical structures and pyrolysis behaviors of three main biopolymers. Then, the controllable preparation of hard carbons using various physicochemical properties of biopolymers at the molecular level is systematically discussed. Furthermore, we highlight present challenges and further opportunities in this field. The Review will guide future research works on the design of sustainable hard carbons and the optimization of battery performance.

关键词： Biomass-derived biopolymers Hard carbons Lithium ion batteries Sodium ion batteries Carbonization

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Edge-enriched MoS2 for kinetics-enhanced potassium storage

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Nano Research 2020年第10期13卷 2763-2769页

作者： Guangshen Jiang Xiaosa Xu Haojie Han Changzhen Qu Hlib Repich Fei Xu Hongqiang Wang State key laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineringShanxi Joint Laboratory of Graphene(NPU)Northwestern Polytechnical UniversityXian 710072China Department of Inorganic Chemistry Technische Universitat DresdenBergstrasse 6601062 DresdenGermany

Potassium-ion batteries (PIBs) hold great promise as alternatives to lithium ion batteries in post-lithium age, while face challenges of slow reaction kinetics induced by the inherent characteristics of large-size K+. We herein show that creating sufficient exposed edges in MoS2 via constructing ordered mesoporous architecture greatly favors for improved kinetics as well as increased reactive sites for K storage. The engineered MoS2 with edge-enriched planes (EE-MoS2) is featured by three-dimensional bicontinuous frameworks with ordered mesopores of ~ 5.0 nm surrounded by thin wall of ~9.0 nm. Importantly, EE-MoS2 permits exposure of enormous edge planes at pore walls, renders its intrinsic layer spacing more accessible for K^+ and accelerates conversion kinetics, thus realizing enhanced capacity and high rate capability. Impressively, EE-MoS2 displays a high reversible charge capacity of 506 mAh·g^−1 at 0.05 A·g^−1, superior cycling capacities of 321 mAh·g^−1 at 1.0 A·g^−1 after 200 cycles and a capacity of 250 mAh·g^−1 at 2.0 A·g^−1, outperforming edge-deficient MoS2 with nonporous bulk structure. This work enlightens the nanoarchitecture design with abundant edges for improving electrochemical properties and provides a paradigm for exploring high-performance PIBs.

关键词： molybdenum disulfide enriched edges potassium-ion batteries kinetics

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Enhancement of oxygen reduction activity and stability via introducing acid-resistant refractory Mo and regulating the near-surface Pt content

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Journal of Energy Chemistry 2020年第12期29卷 246-252页

作者： Shouquan Feng Jiajia Lu Lin Luo Guangfu Qian Jinli Chen Hanna SAbbo Salam JJTitinchi Shibin Yin College of Chemistry and Chemical enginering.School of Physical Science and Technology.key laboratory of New Processing Technology for Nonferrous Metals and Materials State Key Laboratory of Processing for Non Ferrous Metal and Featured MaterialsGuangxi UniversityNanning 530004.GuangxiChina Department of Chemitry University of the Western Cape7535 Cape TownSouth Africa

Although Pt Ni catalyst possesses good oxygen reduction activity, its poor stability is the main obstacle for the commercialization of proton exchange membrane fuel cells(PEMFCs). In this work, we introduce the acid-resistant refractory Mo to enhance the structure stability and modify the electronic structure of Pt in the prepared PtNi catalyst, improving the catalytic activity for oxygen reduction reaction(ORR). In addition, near-surface Pt content in the nanoparticle is also optimized to balance the ORR activity and stability. The electrochemical results show that the alloy formed by Mo and Pt Ni is obviously more stable than the PtNi alloy alone, because the acid-resistant Mo and its oxides effectively prevent the dissolution of Pt. Especially, the Pt3 Ni3 MoN/C exhibits the optimal ORR catalytic performance in O2-saturated 0.1 mol L^(-1) HClO4 aqueous solutions, with mass activity(MA) of 900 m A mg^(-1) Pt at 0.90 V vs. RHE, which is 3.75 times enhancement compared with the commercial Pt/C(240 mA mg^(-1) Pt). After 30 k accelerated durability tests, its MA(690 m A mg^(-1) Pt) is still 2.88 times higher than the pristine Pt/C. This study thus provides a valuable method to design stable ORR catalysts with high efficiency and has great significance for the commercialization of PEMFCs.

关键词： Oxygen reduction reaction Surface platinum content regulate Ternary alloy catalyst Activity Stability

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Investigating the Head Impact Force-Induced Evolution of Hyperphosphorylated Tau Proteins in Brain Tissue Through Mechanical Mesoscale Finite Element Simulation

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Acta Mechanica Solida Sinica 2022年第4期35卷 705-715页

作者： Ge He Lei Fan Shanghai key laboratory of Mechanics in Energy enginering Shanghai Institute of Applied Mathematics and MechanicsSchool of Mechanics and Engineering ScienceShanghai UniversityShanghai 200444China Department of Mechanical Engineering Michigan State UniversityEast LansingMI 48824USA

For human heads that experienced repetitive subconcussive impacts,abnormal accumulation of hyperphosphorylated tau(p-tau)proteins was found in the postmortem brain *** numerically understand the cause–effect relationship between the external force and the microscopic volume change of the p-tau protein,we created a mesoscale finite element model of the multilayer brain tissue containing microscopic voids representing the p-tau *** model was applied under the loading boundary conditions obtained from a larger length scale simulation.A formerly developed internal state variable elastoplasticity model was implemented to describe the constitutive behaviors of gray and white matters,while the cerebrospinal fluid was assumed to be purely *** effects of the initial sizes and distances of p-tau proteins located at four different brain regions(frontal,parietal,temporal and occipital lobes)on their volumetric evolutions were *** is concluded that both the initial sizes and distances of the proteins have more or less(depending on the specific brain region)influential effects on the growth or contraction rate of the p-tau *** p-tau proteins located within the brain tissue at the frontal and occipital lobes are more heavily affected by the frontal impact load compared with those at the parietal and temporal *** summary,the modeling approach presented in this paper provides a strategy for mechanically studying the evolution of p-tau proteins in the brain tissue and gives insight into understanding the correlation between macroscopic force and microstructure change of the brain tissue.

关键词： Traumatic head injury Hyperphosphorylated tau(p-tau)protein Internal state variable Brain tissue

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A gram-scale laboratory synthesis of Annonaceous acetogenin mimic AA005

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Chinese Chemical Letters 2021年第1期32卷 408-412页

作者： Baobao Yu Zhu-Jun Yao State key Laborory of cordnaton Chemisry Jiangu key Laboratoy of Advanced Onganic Materials School of Chemistry and Chemicol Enginering.Nonjing UniversiyNanjing 210023China

AA005(1),a potent anticancer mimicking molecule of natural Annonaceous acetogenin,features a central C_(2)-symmetric triglycol moiety and three stereogenic *** support ongoing animal studies,a scalable 10-step synthesis of AA005(1) has been studied,optimized and accomplished in this work,starting from commercially available economic materials ethylene glycol and(R)-epichlorohydrin.A regio-and stereo-controlled BF_(3)·Et_(2)O-promoted epoxide opening of(R)-epichlorohydrin with ethylene glycol was investigated,optimized and successfully applied to the scalable preparation of the crucial fragment 6 a with C_(2)-*** successive epoxide openings elaborated both two side chains and the whole skeleton with proper nucleophiles and *** and optimization of the reaction sequences finally led to completion of a new multi-gram synthesis ofAA005(1) with satisfactory enantiomeric and diastereomeric purity.

关键词： AA005 Scalable synthesis Annonaceous acetogenin mimic Symmetry Epoxide opening

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Dielectric Manipulated Charge Dynamics in Contact Electrification

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Research 2022年第2期2022卷 295-306页

作者： Kunming Shi Bin Chai Haiyang Zou Daomin Min Shengtao Li Pingkai Jiang Xingyi Huang Depurtment of Polymer Science and Eninering Shanghait Key Laboratoy of Elctrcal lsuaiono and Thermal Aging State Key Laboratory of Metal Matrix CompositesShanghai Hiao Tong UniversiyShanghai 200240China School of Materials Science and enginering Georgia Institute of TechnologyAtlantaGA 30332-0245USA State key laboratory of Eletrical Insulation and Power Equipmenl Xi'an Jiaotong UniversityXi'anShaanxi 710049China

Surface charge density has been demostrated to be sigiantly impacted by the detric properties of ***,the ambiguous physical mechanism of dielectric manipulated charge behavior still restricts the construction of high performance ***,using the atomic force microscopy and Kelvin probe force microscopy,an in situ method was conducted to investigate the contact letrification and charge dynamics on a typical tribomaterial(ie,BaTiOj/PVDF-TrFE nanocomposite)at *** with the characterization of triboelectric device at macroscale,it is found that the number of transferred electrons increases with contact force/area and tends to reach saturation under increased friction *** incorporated high permittivity BaTiO,nanoparticles enhance the capacitance and electron trapping capability of the nanocomposites,eficiently inhibiting the lateral difusion of electrons and improving the output performance of the triboelectric *** decay of the surface potential is observed over monitoring time for all dielectric *** high BaTiO,loadings,more electrons can drift into the bulk and combine with the induced charges on the back electrode,forming a large leakage current and accordingly accelerating the electron ***,the charge trapping/storing and dissipating,as well as the charge attracting properties,should be comprehensively considered in the design of high-performance tribomateras.

关键词： charge trapping dielectric

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