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Constructing oxygen deficiency-rich V_(2)O_(3)@PEDOT cathode for high-performance aqueous zinc-ion batteries

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Rare Metals 2024年第2期43卷 635-646页

作者： Dong-Fei Sun Zi-Juan Wang Tian Tian Xin Yu Dan-Dan Yu Xiao-Zhong Zhou Guo-Fu Ma Zi-Qiang Lei key laboratory of Eco-functional polymer materials of the ministry of education Key Laboratory of Eco-environmental Polymer Materials of Gansu ProvinceSchool of College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou730070China

Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.

关键词： Oxygen defects V_(2)O_(3) PEDOT Electrochemical self-optimization Aqueous zinc-ion batteries

High-speed flexible near-infrared organic photodiode for optical communication

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National Science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin Chen Ruiman Han Hao Qin Zhaoyang Yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng Chen The Centre of Nanoscale Science and Technology and key laboratory of functional polymer materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University State key laboratory of Elemento-Organic Chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

Hexagonal boron nitride based slippery liquid infused porous surface with anti-corrosion, anti-contaminant and anti-icing properties for protecting magnesium alloy

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Chinese Chemical Letters 2024年第4期35卷 532-538页

作者： Wenhao Yan Shuaiya Xue Xuerui Zhao Wei Zhang Jian Li key laboratory of Eco-functional polymer materials of the ministry of education College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070China

In an era where the concept of green development is deeply rooted, magnesium(Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products.Herein, three-dimensional mesopore hollow polypyrrole spheres(MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride(h-BN) lamellae, which allowed the hBN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/hBN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface(SHS). Finally, the slippery liquid infused porous surface(SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.

关键词： Anti-corrosion Mg alloy Hexagon boron nitride Polypyrrole SLIPS

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

Design and synthesis of thiol-terminated imidothioether oligomer as thermally latent hardener and modifier for high-performance epoxy/thiol thermosets

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Science China Chemistry 2024年第2期67卷 632-641页

作者： Xing Liu Jianjun Zhou Shumei Liu Jianqing Zhao School of materials Science and Engineering South China University of TechnologyGuangzhou510640China key Lab Guangdong High Property&functional polymer materials Key Laboratory of Polymer Processing EngineeringMinistry of EducationGuangzhou510640China

Conventional base-catalyzed epoxy/aliphatic thiol systems have a poor storage stability,and are impossible to be one-pot systems.A widely accepted solution is to use the latent catalysts,which are usually insoluble anionic initiators sensitive to impurities and moisture,and have many limitations in practical use.In this work,a soluble thiol-terminated imidothioether oligomer(TPI) was synthesized and used as a latent hardener and modifier to prepare one-pot epoxy/thiol systems without the latent catalysts.The latent behavior and curing mechanism of epoxy systems(EP/TPI series),consisted of bisphenol A diglycidyl ether(DGEBA),pentaerythritol tetrakis(mercaptoacetate)(PETMP) and TPI,were proposed.The thiol exchange reaction between TPI and PETMP preceded the curing reaction of DGEBA,and produced aromatic thiols,which were unreactive at ambient conditions and reacted with DGEBA to form the thermosets at temperatures above 130 ℃.At the loading of 24.4 wt%TPI,the epoxy system(EP/TPI-3) had a shelf life of 13 days and was completely cured within 20 min at 180 ℃.Meanwhile,the catalyst-free curing process of EP/TPI-3 system was insensitive to impurities and moisture.Furthermore,the thermal and mechanical properties of EP/TPI-3 thermoset were simultaneously improved,thereinto,the glass transition temperature,Young's modulus and ultimate tensile strength were increased by 16.7 ℃,12.9%,and 13.6%,respectively,compared with those of the commercial DGEBA/PETMP thermoset.This work shows that TPI has the potential to be a powerful alternative to commercial latent catalysts,and EP/TPI thermosets with high performance have broad application prospects.

关键词： thiol-terminated imidothioether oligomer epoxy systems thiol exchange reaction thermal latency high performance

A Dynamic Covalent Bonding-based Nanoplatform for Intracellular Co-Delivery of Protein Drugs and Chemotherapeutics with Enhanced Anti-Cancer Effect

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Chinese Journal of polymer Science 2024年第5期42卷 559-569,I0005页

作者： Sai-Nan Liu Jia-Hui Meng Li-Yun Cui Hua Chen Lin-Qi Shi Ru-Jiang Ma key laboratory of functional polymer materials of ministry of education Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer MaterialsState Key Laboratory of Medicinal Chemical BiologyFrontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China Haihe laboratory of Sustainable Chemical Transformations Tianjin300192China

Efficient intracellular delivery of protein drugs is critical for protein therapy.The combination of protein drugs with chemotherapeutics represents a promising strategy in enhancing anti-cancer effect.However,co-delivery systems for efficient delivery of these two kinds of drugs are still lacking because of their different properties.Herein,we show a well-designed delivery system based on dynamic covalent bond for efficient intracellular co-delivery of ribonuclease A(RNase A)and doxorubicin(DOX).Two polymers,PEG-b-P(Asp-co-AspDA)and PAE-b-P(Asp-co-AspPBA),and two 2-acetylphenylboronic acid(2-APBA)-functionalized drugs,2-APBA-RNase A and 2-APBA-DOX,self-assemble into mixed-shell nanoparticles(RNase A/DOX@MNPs)via dynamic phenylboronic acid(PBA)-catechol bond between PBA and dopamine(DA)moieties.The PBA-catechol bond endows the nanoparticles with high stability and excellent stimulus-responsive drug release behavior.Under the slight acidic environment at tumor tissue,RNase A/DOX@MNPs are positively charged,promoting their endocytosis.Upon cellular uptake into endosome,further protonation of PAE chains leads to the rupture of endosomes because of the proton sponge effect and the cleavage of PBA-catechol bond promotes the release of two drugs.In cytoplasm,the high level of GSH removed the modification of 2-APBA on drugs.The restored RNase A and DOX show a synergistic and enhanced antic-cancer effect.This system may be a promising platform for intracellular co-delivery of protein drugs and chemotherapeutics.

关键词： Drug co-delivery Combination therapy Dynamic covalent bond

Grain-boundary segregation and grain growth in nanocrystalline substitutional solid solution alloys

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Journal of materials Science & Technology 2024年第1期168卷 239-249页

作者： Fawei Tang Chao Hou Hao Lu Zhi Zhao Xiaoyan Song Faculty of materials and Manufacturing Key Laboratory of Advanced Functional MaterialsMinistry of Education of ChinaBeijing University of TechnologyBeijing 100124China

A model for describing solute segregation at grain boundaries has been developed for substitutional solid solution alloys,which integrates multiple factors from atomic to microstructural scales.A concept of mo-lar Gibbs free energy of segregation was introduced to evaluate the segregating capability of the solute elements in a closed system,through which the influences of grain boundary structure,grain size,ma-terial composition,and external conditions were described.Based on the evaluation of various energy forms related to solute segregation and grain growth processes,the nature of the thermal stabilization of nanograin structures by solute segregation was disclosed.A criterion for the destabilization of nanostruc-tures,which is determined by the competition of the change rates between the molar Gibbs free energy of segregation and the total energy of grain boundaries with grain size,has been proposed.This study provided guideline to achieve high-temperature stability of nanograin structures of solid solution alloys even for the weakly segregating nanocrystalline systems.

关键词： Substitutional solid solution Grain boundary segregation Thermal stabilization Solute concentration Grain size

Multiscale confinement nitridation in molybdenum carbide for efficient hydrogen production

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Journal of Energy Chemistry 2024年第7期94卷 61-69页

作者： Liming Dai Chenchen Fang Xiaoyuan Zhang Xuefeng Xu Xuanxuan Chen Xinyue Zong Xueming Hu Wenyao Zhang Liang Xue Pan Xiong Yongsheng Fu Jingwen Sun Junwu Zhu key laboratory for Soft Chemistry and functional materials Ministry of EducationNanjing University of Science and TechnologyNanjing 210094JiangsuChina

The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.

关键词： Molybdenum carbide Hydrogen evolution reaction Multiscale confinement synthesis Valence band modulation Nitrogen doping

Phosphine-catalyzed acyl-transfer of heteroaryl ketones for the construction of N-fused heterocycles

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Chinese Chemical Letters 2024年第3期35卷 252-256页

作者： Yu Zhang De-Rui Han Dan Ye Hong Lu Hao Wei key laboratory of Synthetic and Natural functional Molecule of the ministry of education College of Chemistry&Materials ScienceNorthwest UniversityXi'an 710069China

An inexpensive phosphine catalyst was used effectively for a transition-metal-free acyl-transfer of N-containing heteroaryl ketones for the rapid synthesis of N-fused heterocycles.The key pre-aromatic spirocyclic intermediate initialized by the single electron transfer(SET)process of Togni's reagentⅡpromoted by the tertiary phosphine resulted in an intriguing and alternative tactic for the cleavage of C–C bonds.By using inexpensive tertiary phosphine as the catalyst,this skeleton-reorganizing approach of N-containing heteroaryl ketones allows a streamlined assembly of complex N-fused heterocycles with broad functional group tolerance.

关键词： Phosphine catalysis Acyl-transfer N-Fused heterocycles C–C bond activation Aromatization