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Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： Lan Wang Peng Jiang Ya-Lin Niu Jun-Peng Cao Tian-Ying Guo Key Laboratory of Functional Polymer materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

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Lithium Sulfur Batteries:Insights from Solvation chemistry to Feasibility Designing Strategies for Practical Applications

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Energy & Environmental materials 2024年第4期7卷 5-27页

作者： Jian Tan Longli Ma Yuan Wang Pengshu Yi Chuming Ye Zhan Fang Zhiheng Li Mingxin Ye Jianfeng Shen Institute of Special materials and Technology Fudan University department of materials Science Fudan University department of chemistry Fudan University

Rechargeable lithium-sulfur (Li-S) batteries,featuring high energy density,low cost,and environmental friendliness,have been dubbed as one of the most promising candidates to replace current commercial rechargeable Li-ion ***,their practical deployment has long been plagued by the infamous"shuttle effect"of soluble Li polysulfides (LiPSs) and the rampant growth of Li dendrites.

关键词： characterization tools design strategies Li–S batteries practical applications solvation chemistry

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Strong and tough chitin hydrogel constructed by dehydration and rehydration strategy

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Nano Research 2024年第9期17卷 8192-8199页

作者： Rui-Rui Liu Li-Bo Mao Shu-Hong Yu Division of Nanomaterials and chemistry Hefei National Research Center for Physical Sciences at the MicroscaleDepartment of ChemistryInstitute of Biomimetic Materials and ChemistryAnhui Engineering Laboratory of Biomimetic MaterialsUniversity of Science and Technology of ChinaHefei 230026China Institute of Innovative materials Department of Materials Science and EngineeringDepartment of ChemistrySouthern University of Science and TechnologyShenzhen 518055China

As a renewable,biocompatible,biodegradable soft material,chitin hydrogels have better advantages in stability,antibacterial activity,antifouling,cost,immunogenicity,and so on than most polymer ***,compared with other widely used polymer hydrogels with high strength and toughness,the practical applications of chitin-based hydrogels have been limited by their weak mechanical properties,such as cartilage repair and meniscus ***,we present the design and fabrication of chitin hydrogels with excellent mechanical strength and toughness by a dehydration and rehydration *** sequential dehydration and rehydration processes,the crystalline domains in the chitin hydrogels can be properly *** optimized crystallinity,the elastic modulus of the chitin hydrogels exceeds all previously reported values,and the fracture toughness is even comparable to some synthetic polymer hydrogels,while maintaining a high-water-content of about 80 wt.%.At the same water content,the mechanical properties of the chitin hydrogels are positively correlated with the hydrogel crystallinity,which proves that the change of mechanical properties of hydrogels is not simply dependent on weight *** hydrogels can be further strengthened by incorporating other biopolymers that are intrinsically weak,which makes the hydrogels promising for applications in fields such as cartilage repair and meniscus ***,the hydrogels enable loading and release of water-soluble and poorly water-soluble *** highly extendable strengthening and toughening strategy of chitin and chitin-based biopolymer hydrogels paves the way for their widely applications.

关键词： chitin hydrogel crystallinity rehydration chemical transformation strong and tough

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Multicolor circularly polarized phosphorescence of axially chiral binuclear platinum(Ⅱ) complexes

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Science China chemistry 2024年第11期67卷 3757-3766页

作者： Jintong Song Rui Zeng Hui Xiao Hailiang Ni Zong-Xiang Xu Haifeng Xiang College of chemistry and materials Science Sichuan Normal University department of chemistry Southern University of Science and Technology College of chemistry Sichuan University

D-A charge transfer, including through-bond charge transfer and through-space charge transfer between two different electron donors（D） and electron acceptors（A）, is a fundamental and powerful tool to tune the optical properties of organic dyes. Herein,we demonstrate a unique strategy to tune phosphorescence and circularly polarized luminescence properties of axially chiral binuclear Pt（Ⅱ） complexes through long-range charge transfer, even though these molecules have two totally identical segments on either side of the chiral core. The presence of axial chirality would break not only the symmetry of molecular structure and π-conjugation system but also the symmetry of charge distribution for long-range charge transfer. These binaphthyl-based Pt（Ⅱ）complexes bearing coordinated atoms far away from chiral axis exhibit no Pt-Pt interactions but colorful concentrationdependent phosphorescence with quantum yield up to 86.4% and could be applied as emitters in highly efficient solutionprocessed organic light-emitting diodes to achieve luminance, luminance efficiency, power efficiency, external quantum efficiency, and asymmetry factor up to 8.94 × 10～3cd m-2, 41.9 cd A-1, 18.8 lm W-1, 12.6% and 2.98 × 10-3, respectively. Therefore,the present work affords a new and simple way to utilize the inherently asymmetric advantage of chirality for the design of D-Abased organic dyes.

关键词： Pt(II) complexes organic light-emitting diodes circularly polarized phosphorescence axial chirality

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Regulation of Lithium-Ion Flux by Nanotopology Lithiophilic Boron-Oxygen Dipole in Solid Polymer Electrolytes for Lithium-Metal Batteries

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Energy & Environmental materials 2024年第4期7卷 74-82页

作者： Manying Cui Hongyang Zhao Yanyang Qin Shishi Zhang Ruxin Zhao Miao Zhang Wei Yu Guoxin Gao Xiaofei Hu Yaqiong Su Kai Xi Shujiang Ding School of chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University department of materials and Environmental chemistry Stockholm University

Inhomogeneous lithium-ion （Li+） deposition is one of the most crucial problems,which severely deteriorates the performance of solid'State lithium metal batteries （LMBs）.Herein,we discovered that covalent organic framework （COF-1） with periodically arranged boron-oxygen dipole lithiophilic sites could directionally guide Li+even deposition in asymmetric solid polymer electrolytes.

关键词： covalent organic framework ion transport regulation lithium metal battery solid polymer electrolyte

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Anisotropic Mechanical Response of Nacre to Heat Treatment Under Indentation:Effect of Structural Orientation

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Journal of Bionic Engineering 2024年第3期21卷 1453-1464页

作者： Simin Liang Yingying Li Hongmei Ji Xiaowu Li department of materials Physics and chemistry School of Materials Science and EngineeringKey Laboratory for Anisotropy and Texture of MaterialsMinistry of EducationNortheastern UniversityShenyang110819China

It is generally considered that heat treatments have a negative impact on the mechanical properties of nacre due to thermal decomposition of the organic ***,the present work investigated the microindentation behavior on fresh and heat-treated nacres from two orthogonal directions,and the results demonstrate that both hardness value and damage tolerance can remain almost unchanged on the cross-section with the organic matrix degeneration,despite a significant deterioration on the platelet *** analyses suggest that the anisotropic response of indentation behavior to heat treatment in nacre is primarily caused by its structural ***,compared with a single layer of irregular interplatelet interfaces in cross-sectional specimens,the multiple layers of parallel interlamellar interfaces in in-plane specimens exhibit a much greater ability to impede indenter-triggered destruction,and heat treatments would reduce the in-plane hardness but nearly have no effect on the cross-sectional ***,the deeper embedding of platelets in cross-sectional specimens enhances their resistance to interface cracking caused by organic matrix degradation at high temperatures,leading to a reduced sensitivity to ***,the indentation behavior of nacre shows different tendencies in response to variations in the organic matrix state along normal and parallel directions.

关键词： Nacre Structural orientation Heat treatment Indentation behavior Organic matrix

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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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Brønsted-acid sites induced photocatalytic cracking of low-polarity polyethylene plastics

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Journal of Energy chemistry 2024年第9期96卷 509-515页

作者： Qianyou Wen Quan Zhang Zhengzheng Liu Huining Wang Shuya Hao Fan Zhang Lijuan Zhang Qing Han Gengfeng Zheng Laboratory of Advanced materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China

Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern ***,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards ***,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline *** to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via *** addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of *** a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.

关键词： Photocatalytic cracking Polyethylene Surface phosphorylation Bronsted-acid site Carbon conversion

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Binding SnO2 Nanoparticles with MoS2 Nanosheets Toward Highly Reversible and Cycle-Stable Lithium/Sodium Storage

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Energy & Environmental materials 2024年第4期7卷 135-142页

作者： Deliang Cheng Wenbiao Zhang Yi Tang Qingsheng Gao Renzong Hu Lichun Yang Min Zhu Institute of Advanced materials Jiangxi Normal University School of materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials South China University of Technology College of chemistry and materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials Fudan University

SnO2,with its high theoretical capacity,abundant resources,and environmental friendliness,is widely regarded as a potential anode material for lithium-ion batteries （LIBs）.Nevertheless,the coarsening of the Sn nanop... 详细信息

关键词： 1 T-MoS2 heterostructure lithium-ion batteries Sn coarsening SnO2

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Liquid-metals-induced formation of MXene/polyacrylamide composite organohydrogels for wearable flexible electronics

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Nano Research 2024年第3期17卷 1913-1922页

作者： Minying Wu Bin Chen Xueliang Fan Tong Ye Yuanyuan Fang Qian Zhang Fangzhou Zhou Yajun Wang Yi Tang department of chemistry Fudan UniversityShanghai 200433China College of chemistry&materials Engineering Wenzhou UniversityWenzhou 325027China

Organohydrogels have demonstrated superior environmental adaptability and frost resistance compared to conventional hydrogels,thereby prompting considerable interests in the development and design of innovative ***,we report an effective one-pot method for fabricating MXene/polyacrylamide(MXene/PAM)composite organohydrogel(MAOH)by employing Ga liquid metals(Ga LMs)as a highly reactive component in the induced free radical polymerization reaction,without the need for additional heating or cross-linking *** synthetic protocol addresses the time-consuming and organic solvent waste concerns associated with traditional solvent displacement methods for organohydrogel *** incorporation of MXene not only highly enhances the conductivity but also confers improved mechanical properties of *** MAOH exhibits excellent environmental adaptability(>7 d),sustained moisture retention,remarkable self-healing capabilities,and outstanding mechanical properties under low temperatures(-20℃).It demonstrates exceptional performance in micro-motion monitoring,rapid response time(125 ms),superior stretchability,and a broad range of strains(0.3%–600%).Therefore,the designed MAOH has great potential for applications in diverse fields such as prosthetics,electronic skin,human–machine interaction,and smart terminals.

关键词： organohydrogels MXene conductivity mechanical properties environmental adaptability

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