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From non-carbon host toward carbon-free lithium-sulfur batteries

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Nano research 2024年第3期17卷 1337-1365页

作者： Yanqi Feng Hui Liu Qiongqiong Lu School of materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Institute of materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China Leibniz Institute for Solid State and materials research(IFW)Dresden e.V. Helmholtzstraβe 2001069 DresdenGermany School of materials&Environment Engineering Chengdu Technological UniversityChengdu 611730China

Lithium-sulfur(Li-S)batteries with advantages of high energy densities(2600 Wh·kg^(-1)/2800 Wh·L^(-1))and sulfur abundance are regarded as promising candidates for next-generation high-energy batteries.However,the conventional carbon host used in sulfur cathodes suffers from poor chemical adsorption towards Li-polysulfides(LPS)in liquid electrolyte and sluggish redox kinetics,leading to low capacity and rate capability.Besides,carbon host used in Li metal anode with the intrinsic property of poor lithiophilicity and high Li-nucleation barrier gives rise to uncontrollable dendrite growth and further battery failure.Therefore,non-carbon hosts with chemical adsorption toward LPS and catalytic activity for accelerating LPS redox conversion as well as lithiophilic property for guiding uniform Li deposition are proposed and demonstrated a high efficiency in both sulfur cathodes and Li metal anodes.In this review,the principle and challenges of Li-S batteries are first presented,then recent work using non-carbon hosts in Li-S batteries is summarized comprehensively,and the mechanism of non-carbon host in improving sulfur utilization and stabilizing Li metal anode is discussed in detail.Furthermore,remaining challenges and outlook on the implementation of non-carbon host for practical carbon-free Li-S batteries are also provided.

关键词： sulfur cathode Li metal anode polysulfides adsorption catalytic effect Li dendrite carbon-free lithium-sulfur batteries

Design and preparation of a crosslinkable,oil-resistant,and bio-based elastomer from fumarate

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Science China Chemistry 2024年第2期67卷 622-631页

作者： Hui Yang Haijun Ji Xinxin Zhou Shihan Yang Liwei Li Chaoying Sun Weiwei Lei Runguo Wang Liqun Zhang Beijing State Key Laboratory of Organic-inorganic Composites&Beijing Laboratory of Biomedical materials Beijing University of Chemical TechnologyBeijing100029China Hubei Key Laboratory of Polymer materials Faculty of Materials Science and EngineeringHubei UniversityWuhan430062China

Poly(diethyl fumarate-co-methoxyethyl acrylate-co-vinyl chloroacetate)(PDEFMV),a novel bio-based elastomer with a saturated structure,was synthesized via redox emulsion polymerization.The glass-transition temperatures of PDEFMV,adjusted through the variation of the diethyl fumarate-to-methoxyethyl acrylate feeding ratio,ranged from-36.1 to-14.8 ℃.The number-average molecular weights of PDEFMV ranged from 384,000 to 46,000 g/mol.In designing the molecular structure,vinyl chloroacetate was used to provide active sites for subsequent vulcanization and crosslinking.The active chlorine groups within the PDEFMV chain reacted with the crosslinking agent trithiocyanuric acid under high temperature and pressure to form a nonsulfur crosslinked three-dimensional network structure.To achieve the desired properties,carbon black(CB,N330) was incorporated to reinforce PDEFMV,leading to the formation of PDEFMV/CB composites.A comprehensive study was conducted on the high-temperature oil resistance of PDEFMV/CB composites.Following immersion in IRM903 oil at temperatures of 150 and 200 ℃ for 72 h,the mass and volume changes in PDEFMV/CB were lower than those observed in commercially available acrylate rubber(AR)/CB,indicating that PDEFMV exhibited superior oil resistance.Furthermore,the aging characteristics and mechanisms of oil resistance in the PDEFMV/CB and AR/CB composites were investigated at different temperatures(150,200,and 250 ℃).The results provide insights into the operational temperature ranges suitable for PDEFMV/CB and offer valuable guidance for potential industrial applications.

关键词： diethyl fumarate molecular design bio-based elastomer solvent-free synthetic route high-temperature oil resistance

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Enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

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Frontiers of Chemical Science and Engineering 2024年第2期18卷 103-112页

作者： Yanqi Feng Hui Liu Xiaoting Liu Qiongqiong Lu School of materials&Environment Engineering Chengdu Technological UniversityChengdu 611730China School of materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Institute of materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China Leibniz Institute for Solid State and materials research(IFW) Dresden e.V.Dresden 01069Germany

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a KV_(3)O_(8)·0.75H_(2)O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K+ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. Moreover, the KV_(3)O_(8)·0.75H_(2)O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g^(-1) and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

关键词： lithium kinetics adsorption

Tetraethylenepentamine-functionalized magnetic mesoporous composites as a novel adsorbent for the removal Cr(III)-ethylenediaminetetraacetic acid in complex solution

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Chinese Journal of Chemical Engineering 2024年第4期68卷 16-26页

作者： Zhi Hu Jiahong Wang Tongtong Sun School of Environmental Science and Engineering Shaanxi University of Science&TechnologyXi'an 710021China Shaanxi Key Laboratory of Green Preparation and Functionalization of inorganic materials Xi'an 710021China

A novel tetraethylenepentamine(TEPA)functionalized magnetic mesoporous silica adsorbent(FNMs/TEPA)was prepared for the adsorption of Cr(III)-ethylenediaminetetraacetic acid(EDTA)from wastewater.The characterization of the prepared adsorbent certified that TEPA was modified onto the magnetic mesoporous silicon(FNMs),while FNMs/TEPA maintained the ordered mesoporous and pristine magnetic properties.The batch adsorption experiments demonstrated that TEPA significantly enhanced the removal capacity of the adsorbent for Cr(III)-EDTA.FNMs/TEPA exhibited an excellent adsorption property(13.84 mg·g^(-1))at pH 4.0.Even in the presence of high concentrations of coexisting ions and organic acids,the adsorption performance of FNMs/TEPA was stable.Experimental characterization and DFT demonstrated that the adsorption of Cr(III)-EDTA was ascribed to the electrostatic interaction,hydrogen bonding,and complexation between Cr(III)-EDTA and amino groups on the adsorbent surface.The analysis of the independent gradient model(IGM)shows that electrostatic interaction is the main mode of action in the adsorption process.Moreover,FNMs/TEPA demonstrated remarkable reusability in three regeneration cycles.These findings indicated that FNMs/TEPA possessed excellent application prospects in the disposal of wastewater containing Cr(III)-EDTA.

关键词： TEPA functionalized magnetic mesoporous silicon Adsorption Cr(III)-EDTA Density functional theory calculations

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Recent progress about transmission electron microscopy characterizations on lithium-ion batteries

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Journal of Energy Chemistry 2024年第8期95卷 39-56页

作者： Yihang Liu Qiuyun Li Ziqiang Wang Institute of materials research Shenzhen International Graduate School Tsinghua University

With the rapid development of portable electronics, new energy vehicles, and smart grids, ion batteries are becoming one of the most widely used energy storage devices, while the safety concern of ion batteries has always been an urgent problem to be solved. To develop a safety-guaranteed battery, the characterization of the internal structure is indispensable, where electron microscopy plays a crucial role. Based on this, this paper summarizes the application of transmission electron microscopy(TEM) in battery safety, further concludes and analyzes the aspects of dendrite growth and solid electrolyte interface(SEI) formation that affect the safety of ion batteries, and emphasizes the importance of electron microscopy in battery safety research and the potential of these techniques to promote the future development of this field. These advanced electron microscopy techniques and their prospects are also discussed.

关键词： Dendrites Electron microscopy characterizations Lithium-ion batteries SEI

Defective MnO2 functional separator coating as effective polysulfide mediators for lithium–sulfur batteries

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Tungsten 2024年第3期6卷 536-543页

作者： Yan-Qi Feng Qiong-Qiong Lu Hui Liu School of materials & Environment Engineering Chengdu Technological University School of materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic Materials Shaanxi University of Science and Technology Institute of materials Henan Key Laboratory of Advanced Conductor Materials Henan Academy of Sciences Institute of materials Chemistry Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V.

Advanced energy storage systems are in urgent need nowadays due to the rising demand in mobile devices and electric vehicles [1]. Lithium–sulfur（Li–S） batteries are intensively studied due to the high theoretical specific capacity(1675 m Ah·g-1) and energy density(2600 Wh·kg-1), as well as natural abundant and environmentally friendly of sulfur.

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Symmetry breaking of highly symmetrical nanoclusters for triggering highly optical activity

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Fundamental research 2024年第1期4卷 63-68页

作者： Xiao Wei Hao Li Honglei Shen Chuanjun Zhou Shuxin Wang Xi Kang Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials.Anhui UniversityHefei 230601China

Developing new approaches to fulfill the enantioseparation of nanocluster racemates and construct cluster-based nanomaterials with optical activity remains highly desired in cluster science,because it is an essential prerequisite for fundamental research and extensive applications of these nanomaterials.We herein propose a strategy termed“active-site exposing and partly re-protecting”to trigger the symmetry breaking of highly symmetrical nanoclusters and to render cluster crystals optically active.The vertex PPh_(3)of the symmetrical Ag_(29)(SSR)_(12)(PPh_(3))_(4)(SSR=1,3-benzenedithiol)nanocluster was firstly dissociated in the presence of counterions with large steric hindrance,and then the exposed Ag active sites of the obtained Ag_(29)(SSR)_(12)nanocluster were partly re-protected by Ag^(+),yielding an Ag_(29)(SSR)_(12)-Ag_(2)nanocluster with a symmetry-breaking construction.Ag_(29)(SSR)_(12)-Ag_(2)followed a chiral crystallization mode,and its crystal displayed strong optical activity,derived from CD and CPL characterizations.Overall,this work presents a new approach(i.e.,active-site exposing and partly re-protecting)for the symmetry breaking of highly symmetrical nanoclusters,the enantioseparation of nanocluster racemates,and the achievement of highly optical activity.

关键词： Atomically precise nanocluster Symmetry breaking Enantioseparation Circularly polarized luminescent Photoluminescence

A novel lead-free relaxor with endotaxial nanostructures for capacitive energy storage

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SusMat 2024年第1期4卷 116-125页

作者： Xiaoyan Dong Tengfei Hu XiaojunWu Jie Yin Zhengqian Fu Jiagang Wu College of materials Science and Engineering Sichuan UniversityChengduP.R.China Analysis and Testing Center for inorganic materials Shanghai Institute of CeramicsChinese Academy of SciencesShanghaiP.R.China

Dielectric capacitors with a fast charging/discharging rate,high power density,and long-term stability are essential components in modern electrical devices.However,miniaturizing and integrating capacitors face a persistent challenge in improving their energy density(W_(rec))to satisfy the specifications of advanced electronic systems and applications.In this work,leveraging phase-field simulations,we judiciously designed a novel lead-free relaxor ferroelectric material for enhanced energy storage performance,featuring flexible distributed weakly polar endotaxial nanostructures(ENs)embedded within a strongly polar fluctuation matrix.The matrix contributes to substantially enhanced polarization under an external electric field,and the randomly dispersed ENs effectively optimize breakdown phase proportion and provide a strong restoring force,which are advantageous in bolstering breakdown strength and minimizing hysteresis.Remarkably,this relaxor ferroelectric system incorporating ENs achieves an exceptionally high W_(rec)value of 10.3 J/cm^(3),accompanied by a large energy storage efficiency(η)of 85.4%.This work introduces a promising avenue for designing new relaxor materials capable of capacitive energy storage with exceptional performance characteristics.

关键词： endotaxial nanostructure energy storage lead-free relaxor ferroelectric

Hollow Metal-Organic Framework/MXene/Nanocellulose Composite Films for Giga/Terahertz Electromagnetic Shielding and Photothermal Conversion

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Nano-Micro Letters 2024年第9期16卷 161-179页

作者： Tian Mai Lei Chen Pei‑Lin Wang Qi Liu Ming‑Guo Ma research Center of Biomass Clean Utilization MOE Engineering Research Center of Forestry Biomass Materials and BioenergyBeijing Key Laboratory of Lignocellulosic ChemistryCollege of Materials Science and TechnologyBeijing Forestry UniversityBeijing 100083People’s Republic of China State Silica-Based materials Laboratory of Anhui Province Bengbu 233000People’s Republic of China

With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.

关键词： Metal-organic frameworks MXene Nanocellulose Electromagnetic shielding Photothermal conversion

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