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Polybenzimidazolium-reinforced polyimide separators to inhibit dendrites for high-security lithium-ion batteries

Science China chemistry 2025年

作者： Guohua Sun Jiaqi Cui Qingsong Zhang Yisong Zhou Xinluo Li Yingying Zhang Zhanao Zhang Xin Zhang Jiantao Fan Pengpeng Li Lianlong Hou Nanjun Chen Hebei key laboratory of Flexible Functional Materials School of Materials Science and Engineering Hebei University of Science and Technology state key laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical Engineering Xiamen University

Lithium dendrite formation poses a significant safety hazard in lithium-ion batteries（LIBs）, severely impeding their widespread adoption and further technological advancements. Here, we present a novel quaternized polybenzimidazolium（q-PBI） to armor polyimide（PI） nanofiber separator（q-PBI@PI）, in which the q-PBI containing lithiophilicity and anionphilicity sites serves as the multifunctional nano-layers to suppress the Li dendrite and reinforce the mechanical properties of PI nanofiber ***, the q-PBI@PI separator displays an unprecedented mechanical strength of 82.8 MPa, significantly outperforming previously reported PI nanofiber membranes（typically below 50.0 MPa）. Besides, we demonstrate that the q-PBI@PI separator simultaneously possesses low nucleation overpotential（59 mV） and exceptional average coulombic efficiency due to the suppression of Li dendrite. Importantly, q-PBI@PI-based Li||Li battery enables a stable Li plating-stripping at 1.0 m A cm-2for600 h. Attributing to these exceptional merits, the armored PI separator-based LIBs display remarkable specific capability and capacity retention. The density function theory calculations reveal that q-PBI is conducive to the desolvation of Li+and can immobilize Li+and PF6-ions near affinity sites of PI nanofibers for inhibiting the formation of Li dendrites. Our work paves a new avenue for the design of next-generation high-performing separators in LIBs.

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Tuning the porosity of {Co12IICo8III（μ3-OH）24（X）}11+ supramolecular frameworks by reaction time for D2/H2 separation

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Science China chemistry 2025年

作者： Zhuozhou Xie Zhu Zhuo Zi-Ang Nan Qing Li Xiufang Li Zi-Xiu Lu Linzhe Lü Jin Liu Luyao Liu Wenjing Wang Wei Wang Daqiang Yuan You-Gui Huang state key laboratory of Structure chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Xiamen key laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of Sciences state key laboratory of physical chemistry of solid surfaces Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University

Systematicly tuning the porosities of porous materials is crucial for targeted gas mixture separation,yet it remains a longstanding *** a common strategy,altering the phenylene ring count in the organic building units has been exploited to adjust pore apertures in metal organic frameworks （MOFs） and covalent organic frameworks （COFs）,resulting in only a stepwise pore size variation of approximately 2.8?.Unlike MOFs and COFs,the porosities for supramolecular assembly frameworks are highly dependent on the packings of the molecular building units in the *** above strategy cannot be applied to supramolecular assembly frameworks and other strategies are required to adjust pore apertures in supramolecular frameworks,especially to achieve porous materials with the optimal pore size for D2/H2separation （～3?）.Here,we successfully modulate the porosity of supramolecular frameworks of[CoII1+12CoIII8L12（μ3-OH）24（X）]1clusters （L=mono-deprotonated 1-iminoisoindole-3-amine,X=ClO?4or Cl?） by controlling the duration of self-assembly *** simply adjusting the reaction time,we obtain three[CoII12CoIII8L12（μ3-OH）24（X）]11+supramolecular frameworks:[CoII12CoIII8（μ3-OH）24（ClO4）L12)]·（Cl）4·（HCO2）7（1）,[CoII12CoIII8L12（μ3-OH）24（Cl）]·（ClOI4）4·（Cl）6·（HCO2）·（H2O）10（2）,and[CoI12CoIII8L12（μ3-OH）24（Cl）]·（Cl）11·（H2O）12（3）.The different stacking patterns of the[CoII12CoIII8L12（μ3-OH）24（X）]11+clusters in these frameworks lead to significantly varied stabilities and *** 1 exhibits permanent porosity with interconnected channels and maintains stability under harsh *** contrast,compound 2 is nearly nonporous,and compound 3 becomes unstable upon *** pores of compound 1 show higher affinity to D2than H2,and the pore aperture diameter of compound 1 （～3.06?） meets the optimal porosity for D2/***,compound 1 demonstrates moderate D2/H2separation at 77 K (retention time:～7 min/g for D2/H2/Ne （10/10/80 vol%） in a flow of 5 mL

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A self-adaptive inorganic in-situ separator by particle crosslinking for nonflammable lithium-ion batteries

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Journal of Energy chemistry 2025年第1期100卷 469-480页

作者： Jiarui Yang Jiuzhou Liu Wenrui Cai Ziyu Zhao Shan Wang Lu He Shanshan Lv Zhiwei Zhu Zhongfeng Ji Guojiang Wen Hua Li Yuanming Zhai Xuewei Fu Wei Yang Yu Wang College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University

All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.

关键词： Silica nanoparticles

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Synthesis and Crystal Structure of Na_2TiO_3

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Chinese Journal of Structural chemistry 2008年第5期27卷 553-557页

作者：毛少瑜任骁侠周朝辉 state key laboratory for physical chemistry of solid surfaces Department of Chemistry Xiamen University

The crystal structure of a sodium titanium oxide Na2TiO3 obtained by high temperature solid state reaction method was determined from single-crystal X-ray diffraction study. The compound crystallizes in the monoclinic system, space group C2/c, Mr = 141.88, a = 9.885（1）, b = 6.4133（8）, c = 5.5048（7） A, β = 115.50（3）°, V = 314.99（7） A^3, Z = 4, Dc = 2.992 g/cm^3, 2 = 0.71073A,μ = 27.80 cm^-1, F（000） = 272, T= 295 K, R = 0.0189 and wR = 0.0512 for 30 variables and 370 contributing unique reflections. The three-dimensional structure in Na2TiO3 is constructed by the TiO（1）4O（2） and NAO（1）3O（2）2 groups. The titanium atoms are grouped in the form of trigonal bipyramid and arranged along the c axis by sharing the edges. The structure is compared with other structures of related A2BO3 compounds.

关键词： synthesis crystal structure X-ray diffraction

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A breakthrough in electrocatalysis of CO2 conversion

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National Science Review 2017年第2期4卷 155-156页

作者： Zhi-You Zhou Shi-Gang Sun state key laboratory of physical chemistry of solid surfaces Xiamen University

Increasing consumption of fossil fuels has resulted in dramatic increase of CO2concentration in the atmosphere,which results in a series of environmental problems such as the greenhouse effect and ocean *** reduction ... 详细信息

关键词： In CO

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Effect of glutathione on in vivo biodistribution and clearance of surface-modified small Pd nanosheets

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Science China chemistry 2015年第11期58卷 1753-1758页

作者： Yizhuan Huang Xiaolan Chen Saige Shi Mei Chen Shaoheng Tang Shiguang Mo Jingping Wei Nanfeng Zheng state key laboratory for physical chemistry of solid surfaces Department of chemistry College of Chemistry and Chemical EngineeringXiamen University

Plasmonic Pd nanosheets have been emerging as promising materials for application in near-infrared(NIR) photothermal therapy(PTT) of cancer. However, animal in mice studies indicated that the original synthesized poly(vinylpyrrolidone)(PVP)-protected small Pd nanosheets(Pd-PVP) and some further surface-modified small Pd nanosheets such as Pd-PEG(SH) easily accumulated in reticuloendothelial system(RES) organs(liver, spleen, etc.) and were difficult to be cleared from these organs quickly. In the work, we surprisingly found that glutathione(GSH) could promote the clearance of surface-modified small Pd nanosheets(e.g. Pd-PVP, Pd-PEG(SH) and Pd-GSH) from the RES organs efficiently. The effects of GSH on the biodistribution and clearance of different surface-modified Pd nanosheets were investigated. Our results indicated that these surface-modified Pd nanosheets with or without GSH added caused no morbidity at target primary organs, and GSH can promote the clearance of different surface-modified Pd nanosheets in the order of Pd-PVP≈Pd-PEG(SH)>Pd-GSH. This study suggests that glutathione could be an attractive reagent for promoting nanomaterials eliminated from the reticuloendothelial systems(RES).

关键词： noble metal nanomaterials glutathione biodistribution renal clearance

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In situ scanning FTIR microscopy and IR imaging of Pt electrode surface towards CO adsorption

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Science China chemistry 1999年第3期42卷 261-267页

作者：孙世刚洪双进陈声培卢国强戴鸿平肖晓银 state key laboratory for physical chemistry of solid surfaces Department of Chemistry Institute of Physical Chemistry Xiamen University Xiamen China

In situ scanning FTIR microscopy was built up for the first time in the present work, which consists of an FTIR apparatus, an IR microscope, an X-Y mapping stage, and the specially designed electrochemical IR cell and computer software. It has been demonstrated that this new space-resolvdin situ IR technique can be used to study vibration properties of micro-area, and to perform IR imaging of electrode surface. The chemical image obtained using this technique for CO adsorption on Pt electrode illustrated, at a space-resolution of 10-2 cm, the inhomogeneity and the distribu-tion of reactivity of micro-area of electrode surface.

关键词： in situ scanning FTIR microscopy reflection spectroscopy IR imaging CO adsorption Pt electrode .

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Copper/cuprous sulfide electrode: preparation and performance

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Science China chemistry 2015年第6期58卷 1039-1043页

作者： Lina Xiao Ding Yuan Pei Li Li Huang Bing-Wei Mao Dongping Zhan state key laboratory for physical chemistry of solid surfaces Department of chemistry College of Chemistry and Chemical Engineering Xiamen University

Cuprous sulfide （Cu2S） is a direct band-gap p-type semiconductor with excellent ionic/electronic hybrid conductivity. Alt- hough Cu/Cu2S/sulfide or polysulfide system is adopted as counter electrode of quantum-dots-sensitized solar cells （QDSSC）, the electrode process is seldom reported. Here, the electrochemical growth of Cu2S film on a copper （Cu） surface, the redox behaviors of sulfide and polysulfide, and the all-in-solid charge-transfer properties of Cu2S film are investigated. It is clarified that the copper electrode simultaneously undergoes an activated process, a membrane growth process, and a redox phase transformation process. The solid charge-transfer capability of CuzS is quantified with a high exchange-current density of 2.27 A/cm2, which elucidates that the Cu/CuzS electrode is a qualified material for counter electrodes of QDSSC. These results aid understanding of the physicochemical mechanism of QDSSC with a polysulfide electrolyte and Cu/Cu2S counter electrode.

关键词： quantum dots sensitized solar cells counter electrode cuprous sulfide film growth

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Ab initio VB Studies of the Ground and Low-lying Excited states of BeH and BH

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Chinese Journal of chemistry 2003年第8期21卷 1005-1010页

作者：廖新丽莫亦荣吴玮张乾二 Department of chemistry State Key Laboratory for Physical Chemistry of Solid Surfaces Center for Theoretical Chemistry Xiamen University

A scheme has been proposed to classify valence bond (VB) wave functions for the calculations of ground and excited states, according to the symmetry properties of one electron orbitals which are involved in the construction of VB wave functions. This scheme is illustrated by the examples of BeH and BH. Ab initio VB computations of these two test molecules in combination with the present classification scheme give reliable results. For example, calculation results show that the state C 2Σ +of BeH is stable, with the bonding energy 0 87 eV and bond length 0 238 nm, which are in good agreement with those obtained by Gerratt et al . The bonding features of ground and low lying excited states of BeH and BH are discussed.

关键词： valence bond theory excited state BeH BH

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Synthetic control of chiral pore surfaces in covalent organic frameworks for enantioselective separation of chiral drugs

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Science China chemistry 2025年

作者： Shiguo Fu Xiaofeng Zhang Kaixuan Wang Linfeng Chen Fan Xia Yong Cui Yan Liu School of chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong University Faculty of Materials Science and chemistry China University of Geosciences

Enantioselective separations of racemates using porous materials are highly attractive and significant in both fundamental research and technological applications. However, achieving controlled chiral pore surfaces to create the necessary driving force for enantiomer discrimination poses a fundamental challenge. Herein, we demonstrate that chiral covalent organic frameworks(COFs) possess the essential characteristics for effective enantioseparations through synthetic control over pore surfaces. We synthesized three 3D chiral COFs (CCOFs) featuring abundant chiral recognition sites on the pore walls via the condensation of enantiopure dialdehyde of 2,2′-dihydroxy-1,1′-binaphthyl and tetraamine. All CCOFs with high stability exhibit an 11-fold interpenetrated framework with tubular open channels, decorated with dihydroxyl or diethoxyl groups. The CCOFs with dihydroxyl groups serve as solid adsorbents for the adsorptive separation and solid-phase extraction of various chiral 1-phenylethanol-derived enantiomers, particularly racemic drugs, achieving up to 98%enantiomeric excess. In contrast, the CCOF with diethoxy groups is unable to resolve the racemates. These CCOF materials can be recycled and reused without any apparent loss of performance. Density functional theory (DFT) calculations reveal that the enantiospecific recognition arises from the well-organized chiral inner sphere and multiple chiral host-guest interactions.

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