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Monophase-homointerface electrodes intrinsically stabilize high-voltage all-solid-state batteries

Science China Chemistry 2024年第5期67卷 1729-1739页

作者： Xiaolin Xiong Xianguo Ma Tianshi Lv Liquan Chen Liumin Suo Beijing National laboratory for condensed matter Physics Institute of PhysicsChinese Academy of ScienceBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The electrochemical stability and contact reliability of heterointerfaces between the solid electrolyte(SE) and electrode are critical for all-solid-state batteries(ASSBs), particularly much more challenging for high-voltage ASSBs, owing to the limited thermodynamically electrochemical window and mechanical inflexibility of SE, aggravating interfacial side reactions and contact failure. Considering all those issues originating from intrinsic heterogeneity in physicochemical features between the cathode material and SE, we are thinking about simplifying the heterointerfaces into a homointerface as a permanent cure to solve all electrochemical-mechanical interfacial failure. Herein, we propose monophase cathodes to construct thermodynamically stable all-in-one homointerfaces in ASS electrodes, removing unstable heterointerfaces by excluding SEs and intrinsically eliminating the Li chemical potential gap to avoid the formation of lithium-depleted space-charge layer and highly resistive mixed ion–electron conductor interphase. Our conception is successfully validated in the layered transition-metal oxide cathodes, which display outstanding stability no matter the MH-LiCoO_(2) cathode charging to 4.7 V or MH-Li_(1.2)Mn_(0.54)Ni_(0.13)-Co_(0.13)O_(2) cathode charging to 5.3 V. It is undeniable that our current version of above-illustrated MH-cathodes would bring out some new challenges for the practical application due to abandoning the SE. However, we believe our work also offers a brandnew direction to ultimately address the electrochemical–mechanical interfacial issues that would be promising for high-energy ASSBs with more discoveries of advanced monophase cathodes in the future.

关键词： monophase-homointerface electrode high-voltage all-solid-state batteries electrochemical-mechanical interfacial issue

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Magnetism of NaYbS_(2):From finite temperatures to ground state

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Science China(Physics,Mechanics & Astronomy) 2024年第10期67卷 92-104页

作者： Weizhen Zhuo Zheng Zhang Mingtai Xie Anmin Zhang Jianting Ji Feng Jin Qingming Zhang School of Physical Science and Technology Lanzhou UniversityLanzhou 730000China Beijing National laboratory for condensed matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

Rare-earth chalcogenide compounds ARECh_(2)(A=alkali or monovalent metal,RE=rare earth,Ch=O,S,Se,Te)are a large family of quantum spin liquid(QSL)candidate ***2is a representative member of the *** key issues on NaYbS_(2),particularly how to determine the highly anisotropic spin Hamiltonian and describe the magnetism at finite temperatures and the ground state,remain to be *** this paper,we conducted an in-depth and comprehensive study on the magnetism of NaYbS_(2) from finite temperatures to the ground ***,we successfully detected three crystalline electric field(CEF)excitation energy levels using low-temperature Raman scattering *** them with the CEF theory and magnetization data,we worked out the CEF parameters,CEF energy levels,and CEF *** further determined a characteristic temperature of~40 K,above which the magnetism is dominated by CEF excitations while below which the spinexchange interactions play a main *** characteristic temperature has been confirmed by the temperature-dependent electron spin resonance(ESR)***-temperature ESR experiments on the dilute magnetic doped crystal of NaYb_(0.1)Lu_(0.9)S_(2) further helped us to determine the accurate ***,we quantitatively obtained the spin-exchange interactions in the spin Hamiltonian by consistently simulating the magnetization and specific heat ***,the above studies allow us to explore the ground state magnetism of NaYbS_(2) by using the density matrix renormalization *** combined numerical calculations and experimental results to demonstrate that the ground state of NaYbS_(2) is a Dirac-like QSL.

关键词： rare-earth chalcogenide anisotropic spin Hamiltonian quantum spin liquid

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Databases of 2D material-substrate interfaces and 2D charged building blocks

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Chinese Physics B 2024年第2期33卷 34-38页

作者：邓俊潘金波杜世萱 Beijing National laboratory for condensed matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physics University of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials laboratory Dongguan 523808China

Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials *** materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this *** van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on *** ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building *** 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI *** the 2D charged building block database,1208 entries from bulk material database are *** of crystal structure,valence state,source,dimension and so on is provided for each entry with a json *** also show its application in designing and searching for new functional layered *** 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://***/10.57760/sciencedb.j00113.00188.

关键词： 2D material-substrate interfaces charged building block database functional-oriented materials design layered materials density functional theory

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Tailoring-compensated ferrimagnetic state and anomalous Hall effect in quaternary Mn–Ru–V–Ga Heusler compounds

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Chinese Physics B 2024年第7期33卷 595-603页

作者：梁瑾静郗学奎王文洪刘永昌 Beijing National laboratory for condensed matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Tiangong University Tianjin 300387China

Cubic Mn_(2)Ru_(x)Ga Heusler compound is a typical example of compensated ferrimagnet with attractive potential for high-density,ultrafast,and low-power spintronic *** the form of epitaxial thin films,Mn_(2)Ru_(x)Ga exhibits high spin polarization and high tunability of compensation temperature by freely changing the Ru content x in a broad range(0.3

关键词： compensated ferrimagnet anomalous Hall effect residual resistivity ratio

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Unlocking the Potential of Poly(butylene succinate)through Incorporation of Vitrimeric Network Based on Dynamic Imine Bonds

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Chinese Journal of Polymer Science 2024年第10期42卷 1414-1424,I0006页

作者： Shan-Song Wu Hui-Juan Lu Yi-Dong Li Shui-Dong Zhang Jian-Bing Zeng Chongqing Key laboratory of soft-matter Material Manufacturing School of Chemistry and Chemical EngineeringSouthwest UniversityChongqing400715China School of Mechanical and Automotive Engineering South China University of TechnologyGuangzhou510640China

Poly(butylene succinate)(PBS)exhibits many advantages,such as renewability,biodegradability,and impressive thermal and mechanical properties,but is limited by the low melt viscosity and strength resulted from the linear *** address this,vitrimeric network was introduced to synthesize PBS vitrimers(PBSVs)based on dynamic imine bonds through melt polymerization of hydroxyl-terminated PBS with vanillin derived imine containing compound and hexamethylene diisocyanate using trimethylolpropane as a crosslinking *** with different crosslinking degrees were synthesized through changing the content of the crosslinking *** effect of crosslinking degree on the thermal,theological,mechanical properties,and stress relaxation behavior of the PBSVs was studied in *** results demonstrated that the melt viscosity,melt strength,and heat resistance were enhanced substantially without obvious depression in crystallizability,thermal stability,and mechanical properties through increasing crosslinking *** addition,the PBSVs exhibit thermal reprocessability with mechanical properties recovered by more than 90%even after processing for three ***,PBSV with improved melt properties shows significantly improved foamability compared to commercial *** research contributes to the advancement of polymer technology by successfully developing PBS vitrimers with improved properties,showcasing their potential applications in sustainable and biodegradable materials.

关键词： Poly(butylene succinate) Vitrimer Imine bonds Foamability

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Effect of trace oxygen on plasma nitriding of titanium foil

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Chinese Physics B 2024年第6期33卷 548-551页

作者：周海涛熊希雅马可欣罗炳威罗飞申承民 Beijing Institute of Aeronautical Materials Aero Engine Corporation of ChinaBeijing 100095China Beijing National laboratory of condensed matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

Titanium nitride films are prepared by plasma enhanced chemical vapor deposition method on titanium foil using N_(2) as precursor. In order to evaluate the effect of oxygen on the growth of titanium nitride films, a small amount of O_(2) is introduced into the preparation process. The study indicates that trace O_(2) addition into the reaction chamber gives rise to significant changes on the color and micro-morphology of the foil, featuring dense and long nano-wires. The as-synthesized nanostructures are characterized by various methods and identified as TiN, Ti_(2) N, and TiO_(2) respectively. Moreover, the experiment results show that oxide nanowire has a high degree of crystallinity and the nitrides present specific orientation relationships with the titanium matrix.

关键词： nitride oxide nanostructure crystalline plasma-enhanced chemical vapor deposition system(PECVD)

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Synthesis of poly(thiourethane-alt-thioester)by alternating ring-opening copolymerization of N-thiocarboxyanhydrides and episulfides

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Science China Chemistry 2024年第9期67卷 3091-3097页

作者： Wei Xiong Tianjun Yue Haiwang Lai Chunyan Lyu Weimin Ren Hua Lu Beijing National laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key laboratory of Fine Chemicals Dalian University of TechnologyDalian 116081China

Polythiourethanes(PTU)and polythioesters(PTE)derived from renewable sources are emerging sustainable polymers for their excellent degradability and ***,P(TU-alt-TE)copolymers have been rare and challenging to ***,we report the efficient synthesis of novel P(TU-alt-TE)copolymers via the alternating copolymerization of N-thiocarboxyanhydrides(NTA)/episufides(ES)and provide mechanistic insight into the alternating chain propagation process via density functional theory(DFT)*** incorporation of ESs into traditional peptide backbone is capable of adjusting the glass transition temperature below thermal decomposition temperature,which confers better thermal processability by regulating the rigidity of the backbone and the hydrogen bond interaction among the polymer *** PTUs with tailored properties are accessible by altering the feeding ratio of NTAs and(bifunctional)***,the thiourethane in the backbone can endow interesting underwater adhesion properties to the *** the broad scope of NTA and ES monomers,this method is expected to provide a promising and general route to a wide range of P(TU-alt-TE)copolymers with diverse properties.

关键词： poly(thiourethane-alt-thioester) alternating ring-opening copolymerization N-thiocarboxyanhydrides episulfides

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A pseudoclassical theory for the wavepacket dynamics of the kicked rotor model

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Science China(Physics,Mechanics & Astronomy) 2024年第3期67卷 34-43页

作者： Zhixing Zou Jiao Wang Department of Physics and Key laboratory of Low Dimensional condensed matter Physics(Department of Education of Fujian Province) Xiamen UniversityXiamen 361005China Lanzhou Center for Theoretical Physics Lanzhou UniversityLanzhou 730000China

In this study, we propose a generalized pseudoclassical theory for the kicked rotor model in an attempt to discern the footprints of the classical dynamics in the deep quantum regime. Compared with the previous pseudoclassical theory that applies only in the neighborhoods of the lowest two quantum resonances, the proposed theory is applicable in the neighborhoods of all quantum resonances in principle by considering the quantum effect of the free rotation at a quantum resonance. In particular, it is confirmed by simulations that the quantum wavepacket dynamics can be successfully forecasted based on the generalized pseudoclassical dynamics, offering an intriguing example where it is feasible to bridge the dynamics in the deep quantum regime to the classical dynamics. The application of the generalized pseudoclassical theory to the PT-symmetric kicked rotor is also discussed.

关键词： quantum-classical correspondence kicked rotor model pseudoclassical theory wavepacket dynamics

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Mutation in a non-force-bearing region of protein L influences force-dependent unfolding behavior

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Chinese Physics B 2024年第7期33卷 624-629页

作者：蒋环杰王艳伟陈家媛胡丹潘海郭子龙陈虎 Department of Physics Wenzhou UniversityWenzhou 325035China Center of Biomedical Physics Wenzhou InstituteUniversity of Chinese Academy of SciencesWenzhou 325000China Research Institute for Biomimetics and soft matter Fujian Provincial Key Laboratory for Soft Functional Materials ResearchDepartment of PhysicsXiamen UniversityXiamen 361005China

Single-molecule magnetic tweezers(MTs) have revealed multiple transition barriers along the unfolding pathway of several two-state proteins, such as GB1 and Csp. In this study, we utilized MTs to measure the force-dependent folding and unfolding rates of both protein L(PLWT) and its Y47W mutant(PLY47W) where the mutation point is not at the force-bearing β-strands. The measurements were conducted within a force range of 3–120 pN. Notably, the unfolding rates of both PLWT and PWY47W exhibit distinct force sensitivities below 50 pN and above 60 pN, implying a two-barrier free energy landscape. Both PLWT and PLY47W share the same force-dependent folding rate and the same transition barriers,but the unfolding rate of PLY47W is faster than that of PLWT. Our finding demonstrates that the residue outside of the force-bearing region will also affect the force-induced unfolding dynamics.

关键词： protein folding magnetic tweezers protein L

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Polyolefin vitrimers bearing acetoacetate functionality

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Science China Chemistry 2024年第11期67卷 3861-3867页

作者： Zihao Wang Yue Liu Wenmin Pang Ao Chen Min Chen Chinese Academy of Sciences (CAS) Key laboratory of soft matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University

Polyolefin vitrimers are polymer networks bearing reversible covalent crosslinking points, enabling them to be reprocessed and recycled. In this contribution, a series of polyolefin vitrimers were designed based on the acetoacetate-functionalized polyolefin copolymers, which were produced through the direct copolymerization of ethylene with polar comonomers using a phosphinesulfonate palladium catalyst. The pendant acetoacetate group could mediate several characteristic reactions, such as the Michael addition reaction, ketone-amine condensation and metal coordination reaction. As such, structurally adjustable polyolefin vitrimers can be accessed by introducing various dynamic crosslinking bonds, including disulfide exchange, transamination of vinylogous urethane and labile metal coordination bond. The utilization of different crosslinking reactions and the mole ratio of crosslinkers significantly impact the material properties of the resultant polymers. Specifically, the generated polyolefin vitrimers demonstrated excellent reprocessability and closed-loop recycling properties. The study in this work provides an efficient strategy to access various polyolefin vitrimers.

关键词： polyolefin vitrimers acetoacetate group polar monomer olefin copolymerization

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