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A bifunctional POM-based Cu-viologen complex with mixed octamolybdate clusters for rapid oxidation desulfurization and effective photogeneration of hydrogen

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Rare Metals 2024年第1期43卷 236-246页

作者： lin Yang Zhong Zhang Chao-Nan Zhang xiu-li wang College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of liaoning Province for Conversion Materials of Solar Cell Bohai UniversityJinzhou 121013China

The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy ***,a novel bifunctional [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)-based Cu-viologen complex H_(4)[Cu_(2)~ⅠCl_(2)(Hbcbpy)_(4)] [α-Mo_(8)O_(26)] [β-Mo8O_(26)]·H_(2)O(BHU-2,Hbcbpy=1-(4-carboxybenzyl)-4,4'-bipyridinium) was synthesized and characterized by single-crystal X-ray diffraction(XRD),infrared radiation spectra,powder X-ray diffraction(PXRD) and X-ray photoelectron spectroscopy(XPS) *** structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu_(2)ⅠCl_(2)(Hbcbpy)_(4)]^(4+).BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen *** room temperature,BHU-2 can catalyze 96% conversion of methyl phenyl sulfide with 98% selectivity,and the process obeys the pseudo-first-order reaction kinetic with the half-life of9.6 *** notorious 2-chloroethyl ethyl sulfide can achieve 99% conversion with 98% selectivity within only1 min at the presence of BHU-2,and the turnover frequency(TOF) is up to 7400 h^(-1).BHU-2 also exhibits high catalytic activity for the oxidation of other aromatic and aliphatic thioethers within short time at room ***,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H_(2) evolution rate of 1677.85 μmol·g^(-1)·h^(-1) within 10 ***,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.

关键词： Polyoxometalate Metal-organic complex Viologen Oxidation desulfurization Photocatalytic hydrogen production

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A homopolymolybdate-supported plate-like 2D cobalt network constructed from a new pyrazole-amide-pyridyl ligand: highly electrochemical activity in both capacitive performance and the detection of Cr(Ⅵ)

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Tungsten 2024年第2期6卷 422-427页

作者： xiu-li wang Yong-Zhen Chen Zhi-Han Chang Yu-Chun lin Jing-Yi Ma College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of liaoning Province for Conversion Materials of Solar Cell Jinzhou 121013China

By employing a new semi-rigid pyrazole-amide-derived bis(pyridyl)ligand[N,N'-bis(4-picolylamine)-1-hydropyrazole(4-dpap)],a new homopolymolybdate-based two-dimensional(2D)plate-like complex[Co(4-dpap)(H_(2)O)(β-Mo_(8)O_(2)6)1/2](1)has been prepared under solvothermal condition and structurally ***β-Mo_(8)anions are fi xed between the 2D metal–organic networks[Co(4-dpap)(H_(2)O)]n 2n+via hydrogen-bonding *** 1 possesses satisfactory specifi c capacitance of 1512.4 F·g^(−1)(current density:1 A·g^(−1))and good cycling stability(90.8%after 1000 cycles).Moreover,1 represents a promising amperometric sensor for measurement of Cr(Ⅵ)with low detection limit(0.042μmol·L^(−1))and high *** insertion ofβ-Mo_(8)anions between the unique 2D metal−organic networks improves the active area of polyoxometalates,which further promotes electrochemical performance.

关键词： Homopolymolybdate Metal–organic network Pyrazole-amide-derived bis(pyridyl)ligand Supercapacitor Electrochemical sensor

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Reversibly Cross-linking Polyimide and Cyclophosphazene Toward Closed-Loop Recyclable Plastics with High Mechanical Strength,Excellent Flame Retardancy,and Chemical Resistance

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CCS Chemistry 2024年第4期6卷 976-987页

作者： Tingting Guan Xiaohan wang Xi Zhao Xingyuan Lu xiu-li wang Yu-Zhong wang Junqi Sun State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012 The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064

Traditional flame-retardant plastics are technically difficult to chemically *** development of newtypes of flame-retardant plastics that are intrinsically capable of being closed-loop recycled and are sufficiently robust and stable to satisfy their practical application is urgently *** this study,closed-loop recyclable flame-retardant plastics with high mechanical strength and excellent chemical resistance are fabricated by cross-linking amino-terminated polyimide(PI-NH_(2))and aldehyde-terminated cyclophosphazene(CP-CHO)with imine *** resultant flame-retardant plastic,which is denoted as PI-CP,exhibits a tensile strength of∼115.6 MPa,Young’s modulus of∼2.5 GPa,and glass transition temperature of 316°*** the PI-CP plastic,the imine bonds are isolated within hydrophobic microenvironments generated by the rigid and hydrophobic polyimide chains and the benzene ring of *** a result,the PI-CP plastics are highly stable in highly acidic and basic aqueous solutions and other commonly used organic *** PI-CP plastic shows outstanding flame retardancy with a limiting oxygen index value of 48.8%.More importantly,the PI-CP plastic can be depolymerized to generate the original PI-NH_(2)and CPCHO monomers in high yields(∼97%)and *** recovered monomers can be used to refabricate the original plastics,establishing highly efficient polymer-monomer-polymer circulation and a sustainable plastics economy.

关键词： closed-loop recyclable plastics recyclable polymers reversibly cross-linked polymers flame retardancy supramolecular polymers

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Thermotolerant and fireproof gel polymer electrolyte toward high-performance and safe lithium-ion battery

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Journal of Energy Chemistry 2022年第2期31卷 9-18页

作者： Man-Cheng Long Ting wang Ping-Hui Duan You Gao xiu-li wang Gang Wu Yu-Zhong wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064China

Poly(ethylene oxide)(PEO)and its derivatives based gel polymer electrolytes(GPEs)are severely limited in advanced and safe lithium-ion batteries(liBs)owing to the intrinsically high flammability of liquid electrolytes and *** adding flame retardants to the GPEs can suppress their flammability and thus improve the safety of liBs,but results in deteriorative electrochemical ***,a novel GPE with chemically bonded flame retardant(*** vinylphosphonate)in cross-linked polyethylene glycol diacrylate matrix,featuring both high-safety and high-performance,is *** as-prepared GPE storing the commercial 1 mol L^(-1) liPF6 electrolyte resists high temperature of 200℃and cannot be ignited as well as possesses a high ionic conductivity(0.60 m S cm^(-1))and good compatibility with ***,the liFePO_(4)/li battery with this GPE delivers a satisfactory capacity of 142.2 m A h g^(-1) and a superior cycling performance with a capacity retention of 96.3%and a coulombic efficiency of close to 100%for 350 cycles at 0.2 C under ambient ***,the battery can achieve steady charge–discharge for 100 cycles with a coulombic efficiency of 99.5%at 1 C under 80℃and run normally even at a high temperature of 150℃or under the exposure to butane *** scanning calorimetry manifests significantly improved battery safety compared to commercial battery *** work provides a new pathway for developing next-generation advanced liBs with enhanced performance and high safety.

关键词： Gel polymer electrolyte Poly(ethylene oxide) Flame retardant Vinylphosphonate lithium-ion batteries

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A bio-based epoxy resin derived from p-hydroxycinnamic acid with high mechanical properties and flame retardancy

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Chinese Chemical Letters 2022年第11期33卷 4912-4917页

作者： Xin Song Ze-Peng Deng Chun-Bo li Fei Song xiu-li wang li Chen De-Ming Guo Yu-Zhong wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064China

Recent advances in epoxy resins have been forward to achieving high mechanical performance,thermal stability,and flame ***,seeking sustainable bio-based epoxy precursors and avoiding introduction of additional flame-retardant agents are still of increasing *** we report the synthesis of p-hydroxycinnamic acid-derived epoxy monomer(HCA-EP)via a simple one-step reaction,and the HCA-EP can be cured with 4,4′-diaminodiphenylmethane(DDM)to prepare epoxy *** with the typical petroleum-based epoxy resin,bisphenol A epoxy resin,the HCA-EP-DDM shows a relatively high glass transition temperature(192.9℃)and impressive mechanical properties(tensile strength of 98.3 MPa and flexural strength of 158.9 MPa).Furthermore,the HCA-EP-DDM passes the V-1 flammability rating in UL-94 test and presents the limiting oxygen index of 32.6%.Notably,its char yield is as high as 31.6%under N_(2),and the peak heat rate release is 60%lower than that of bisphenol A epoxy *** findings provide a simple way of using p-hydroxycinnamic acid instead of bisphenol A to construct high-performance bio-based thermosets.

关键词： Epoxy resin Bio-based p-Hydroxycinnamic acid Mechanical performance Intrinsic flame retardancy

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Multifunctional robust aerogel separator towards high-temperature,large-rate,long-cycle lithium-ion batteries

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Chinese Chemical Letters 2023年第5期34卷 530-534页

作者： Mei-Chen liu Hui-Jun Chen Gang Wu xiu-li wang Yu-Zhong wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064China

Separators is indispensable for the normal operation of lithium-ion batteries(liBs).However,the widely used commercial polyolefin separators have some inherent deficiencies such as poor thermotolerance,high inflammability and inferior electrolyte wettability,which restrict their further applications of the advanced and safe ***,we design a novel thermotolerant(a shrinkage percentage of 0%at 300℃)and flame retarded aerogel separator consisting of aramid nanofibers(ANFs).Because of its high porosity(86.5%±6.1%)and excellent electrolyte uptake(695%),the ANFs aerogel separator has an ionic conductivity of 1.04 mS/cm and a high lithium-ion transference number(0.67),which can endow liBs with outstanding rate performance and superior cycling ***,the ANFs aerogel separator-based batteries possess a discharge specific capacity of 102 m Ah/g with a capacity retention of 90.7%and a Coulombic efficiency of 99.3%after 600 cycles at 5 *** addition,under an operated temperature of 90℃,the battery with ANFs aerogel separator can still conduct the very steady chargedischarge,presenting a capacity retention of 90.1%and a Coulombic efficiency of 99.6%after 200 cycles at 3 ***,the separator can probably serve as a potential candidate for application to advanced and safe liBs.

关键词： Aramid nanofibers Aerogel separator lithium-ion batteries High performance Safety

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Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries

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能源化学:英文版 2023年第8期83卷 239-246,I0008页

作者： Qing-Song liu Yi-Zhou Quan Mei-Chen liu Guo-Rui Zhu xiu-li wang Gang Wu Yu-Zhong wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064SichuanChina

The rapid development and widespread application of lithium-ion batteries(liBs) have increased demand for high-safety and high-performance liBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on liBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate(BMOP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity,high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for liBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance liBs.

关键词： Multifunctional additives Electrode compatibility Solid electrolyte interface Solvation structure lithium-ion batteries

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Flame-retardant oligomeric electrolyte additive for self-extinguishing and highly-stable lithium-ion batteries:Beyond small molecules

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Journal of Energy Chemistry 2023年第9期84卷 374-384页

作者： Yi-Zhou Quan Qing-Song liu Mei-Chen liu Guo-Rui Zhu Gang Wu xiu-li wang Yu-Zhong wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064SichuanChina

Preparing both safe and high-performance lithium-ion batteries(liBs) based on commonly used commercial electrolytes is highly desirable,yet *** overcome the poor compatibility of conventional small-molecular flame-retardants as electrolyte additives for safe liBs with graphite anodes,in this study,we propose and design a novel low-cost flame-retardant oligomer that achieves an accurate and complete reconciliation of fire safety and electrochemical performance in *** to the integration of phosphonate units and polyethylene glycol(PEG) chains,this oligomer,which is a phosphonatecontaining PEG-based oligomer(PPO),not only endows commercial electrolytes with excellent flame retardancy but also helps stabilize the electrodes and li-ion ***,adding 15 wt% of PPO can reduce 70% of the self-extinguishing time and 54% of total heat release for commercial ***,liFePO_(4)/lithium and graphite/lithium cells as well as liFePO_(4)/graphite pouch full cells exhibit good long-term cycling stability.

关键词： Flame-retardant oligomer Safety Compatibility Graphite anodes lithium-ion batteries

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Design and synthesis of liquid crystal copolyesters with high-frequency low dielectric loss and inherent flame retardancy

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Chinese Chemical Letters 2023年第5期34卷 621-625页

作者： Shi-Yu Zhang Teng Fu Yue Gong De-Ming Guo xiu-li wang Yu-Zhong wang State Key Laboratory of Polymer Materials Engineering The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric MaterialsNational Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)College of ChemistrySichuan UniversityChengdu 610064China

Ultra-low dielectric loss(Df)and low dielectric constant(Dk)materials are urgently required in highspeed and large-capacity transmission,in which the wholly aromatic liquid crystal polymer(LCP)has gained attention due to its excellent dielectric ***,the relationship between molecular structure and dielectric properties is still not *** this study,two copolyesters containing phenyl or naphthyl structures are synthesized,as well as the effects of benzene and naphthalene mesogens on dielectric properties are *** synthesized copolyesters containing naphthalene structure have good comprehensive properties with high thermal stability(T_(5%)=479℃ and T_g=195-216℃),inherent flame retardance(LOI=33.0-35.0 and UL-94 V-0 level at 0.8 mm),low Dk(2.9-3.0@10 GHz)and low Df(0.0027-0.0047@10 GHz).Naphthalene mesogen can reduce the dielectric loss more significantly than benzene at high frequency by reducing the density and mobility of polarizable groups,which leads to the effectively limited dipole polarization in ***,we proposed a new strategy for designing low Dk and low Df materials.

关键词： liquid crystal polymer Low dielectric loss Low dielectric constant Naphthalene structure Flame retardant

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Oral Microbiota:A New Insight into Cancer Progression,Diagnosis and Treatment

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Phenomics 2023年第5期3卷 535-547页

作者： xiu-li wang Hua-Wen Xu Ning-Ning liu State Key Laboratory of Systems Medicine for Cancer Center for Single-Cell OmicsSchool of Public HealthSchool of MedicineShanghai Jiao Tong UniversityShanghai 200025China

The polymorphic microbiome has been defined as one of the“Hallmarks of Cancer”.Extensive studies have now uncovered the role of oral microbiota in cancer development and ***,fungi,archaea,and viruses in the oral cavity interact dynamically with the oral microenvironment to maintain the oral micro-ecological *** complex interaction is influenced by many factors,such as maternal transmission,personal factors and environmental *** of oral microbiota can disturbed this host-microbiota interaction,leading to systemic *** studies have shown the potential associations between oral microbiota and a variety of ***,the underlying mechanisms and therapeutic insights are still poorly *** this review,we mainly focus on the following aspects:(1)the factors affect oral microbiota composition and function;(2)the interaction between microenvironment and oral microbiota;(3)the role of multi-kingdom oral microbiota in human health;(4)the potential underlying mechanisms and therapeutic benefits of oral microbiota against ***,we aim to describe the impact of oral microbiota on cancer progression and provide novel therapeutic insights into cancer prevention and treatment by targeting oral microbiota.

关键词： Oral microbiota Cancer Cancer diagnosis Tumor therapy

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