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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 *** combination of protein drugs with chemotherapeutics represents a promising strategy in enhancing anti-cancer ***,co-delivery systems for efficient delivery of these two kinds of drugs are still lacking because of their different ***,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)*** PBA-catechol bond endows the nanoparticles with high stability and excellent stimulus-responsive drug release *** the slight acidic environment at tumor tissue,RNase A/DOX@MNPs are positively charged,promoting their *** 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 *** cytoplasm,the high level of GSH removed the modification of 2-APBA on *** restored RNase A and DOX show a synergistic and enhanced antic-cancer *** 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

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Defect spinel oxides for electrocatalytic reduction reactions

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Nano Research 2024年第5期17卷 3547-3570页

作者： Zhijuan Liu Jinyu Guo Lu-yu Liu Fen Wang Zhijie Kong Yanyong Wang Henan Key laboratory of Crystalline Molecular Functional materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsKey Laboratory of Special Environmental Functional Materials(Zhengzhou University)Ministry of EducationGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China State Key laboratory of Chem/Bio-sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Electrocatalytic reduction reactions play a crucial role in electrochemical energy conversion and storage technology,which are emerging technologies to ameliorate environmental *** oxides are widely explored in electrocatalytic oxidation reactions but have a poor intrinsic ability to reduction reactions,making their electrocatalytic ability less *** improve this,defect engineering is a valuable method for regulating the electronic structure and coordination ***,this manuscript discusses the use of defect spinel oxides in electrocatalytic reduction reactions,including the different types of defects,construction methods,and characterization *** also outlines the various applications of defect spinel oxides in different electrocatalytic reduction ***,it goes over the challenges and future outlooks for defect *** review aims to thoroughly explain how defect spinels work in electrocatalytic reduction reactions and serve as a helpful guide for creating effective electrocatalysts.

关键词： defect spinel oxides electrochemical reduction reactions electrocatalytic mechanism dynamic evolution

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Boosting thermal stability and crystallization of closed-loop-recyclable biodegradable poly(p-dioxanone) by end-group regulation

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Science China chemistry 2024年第2期67卷 642-651页

作者： Jin Lei Zhu-Xin Gui Wan-Ting Xiong Gang Wu Si-Chong Chen 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 UniversityChengdu610064China

A chemically closed-loop-recyclable biodegradable polymer,poly(p-dioxanone)(PPDO),is one of the ideal candidates for single-use plastic products due to its suitability for different application ***,when PPDO wastes can be collected,its monomer p-dioxanone(PDO) will be obtained through chemical recycling of these wastes;when cannot be collected,the wastes are able to be biodegraded into harmless ***,unsatisfied thermal stability and low crystallization rate of PPDO restrict its wider ***,based on end-group regulation,we simultaneously realized the significant enhancement of thermal stability and crystallization of PPDO through the simple melt processing with tributyl phosphite(TBP) or triphenyl phosphite(TPP).The model reactions were conducted to investigate the reaction mechanism and theoretical products during the preparation of PPDO/phosphite *** kinds of phosphites were proved to act as the end-capped reagent and chain extender in the melt processing,while TBP presented better *** a result,the activation energy of thermal decomposition was largely elevated,and the unprecedented T_(5%)(the temperature at a weight loss of 5%) and Tmax(the temperature at a maximum rate of weight loss) of PPDO were obtained,i.e.,T_(5%)of ~330 ℃ and Tmaxof ~385 ℃ in N_(2) atmosphere,T_(5%)of ~240 ℃ and Tmaxof ~317 ℃ in air atmosphere,***,the increased crystallization rate,crystallinity,crystalline orderliness,and realizable monomer recovery(yield >90%,purity >99.9%) of PPDO/phosphite compounds were confirmed.

关键词： poly(p-dioxanone) phosphite thermal stability crystallization end-group regulation

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Chiral thermally activated delayed fluorescence materials for circularly polarized organic light-emitting diodes

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Science China chemistry 2024年第4期67卷 1097-1116页

作者： Li Yuan Yi-Pin Zhang You-Xuan Zheng State Key laboratory of Coordination chemistry Collaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chirality is an important natural characteristic of organic molecules,and chiral organic molecules have shown extensive application in areas such as pharmaceutical development and material *** from the ability to achieve circularly polarized luminescence(CPL),chiral luminescent materials have shown potential applications in anti-glare display,optical communication and,3D display,*** to the ability to harvest both singlet and triplet excitons by a fast reverse intersystem crossing process without involving noble metals,chiral thermally activated delayed fluorescence(TADF)materials with point chirality,axial chirality,planar chirality and helical chirality are regarded as the state-of-the-art materials for circularly polarized organic light-emitting diodes(CP-OLEDs).In recent years,the chiral TADF materials and CP-OLEDs have rapidly developed,but unfortunately,the dissymmetry factors(g)are far from the requirement of practical *** ideal emitters and devices should have both high efficiency and a g factor,or at least a balance between these two *** review gives an overview of recent progress in chiral TADF materials,with a particular focus on the chiral skeleton,CPL property and device ***,the molecular design concept,device structure and methods to improve the g factors of chiral materials and CP-OLEDs are also discussed.

关键词： chiral thermally activated delayed fluorescence material chiral skeleton circularly polarized luminescence circularly polarized organic light-emitting diodes dissymmetry factor

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Waste acid recovery utilizing monovalent cation permselective membranes through selective electrodialysis

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Chinese Journal of Chemical Engineering 2024年第7期71卷 45-57页

作者： Yanran Zhu Yue Zhou Qian Chen Rongqiang Fu Zhaoming Liu Liang Ge Tongwen Xu Anhui Provincial Engineering laboratory of Functional Membrane materials and Technology Department of Applied ChemistrySchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China Key laboratory of Charged Polymeric Membrane materials of Shandong Province Shandong Tianwei Membrane Technology Co.Ltd.Weifang 261000China

Selective electrodialysis(SED)has surfaced as a highly promising membrane separation technique in the realm of acid recovery owing to its ability to effectively separate monovalent ions through the utilization of a potential ***,the current SED process is limited by conventional commercial monovalent cation permselective membranes(MCPMs).This study systematically investigates the use of an independently developed MCPM in the SED process for acid *** factors such as current density,volume ratio,initial ion concentration,and waste acid systems are *** independently developed MCPM offers several advantages over the commercial monovalent selective cation-exchange membrane(CIMS),including higher recovered acid concentration,better ion flux ratio,improved acid recovery efficiency,increased recovered acid purity,and higher current *** SED process with the MCPM achieves a recovered acid of 95.9%and a concentration of 2.3 mol·L^(–1) in the HCl/FeCl_(2) system,when a current density of 20 mA·cm^(-2) and a volume ratio of 1:2 are ***,in the H_(2)SO_(4)/FeSO_(4) system,a purity of over 99%and a concentration of 2.1 mol·L^(–1) can be achieved in the recovered *** study thoroughly examines the impact of operation conditions on acid recovery performance in the SED *** independently developed MCPM demonstrates outstanding acid recovery performance,highlighting its potential for future commercial utilization.

关键词： Selective electrodialysis Wastewater Monovalent cation permselective membranes Separation Recovery

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MOF-derived Se doped MnS/Ti_(3)C_(2)T_(x) as cathode and Zn-Ti_(3)C_(2)T_(x) membrane as anode for rocking-chair zinc-ion battery

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Nano Research 2024年第4期17卷 2781-2789页

作者： Kaisheng Sun Zemao Xiao Yunfei Shen Heng Lv Jianpeng Zhu Jianxiang Pang Yang Zheng Wenwen Kong Long Chen School of chemistry and Chemical Engineering/State Key laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003China CAS Key laboratory of Functional materials and Devices for Special Environments Xinjiang Key Laboratory of Electronic Information Materials and DevicesCenter of Materials Science and Optoelectronics EngineeringXinjiang Technical Institute of Physics and Chemistry of CASUrumqi 830011China

Mn-based zinc ion battery has the advantages of low cost and high performance,which makes it the promising energy storage ***,the poor conductivity and the agglomeration in the synthesis process of manganese-based materials restrict the performance of ***,the Se-doped MnS/Ti_(3)C_(2)T_(x)(Se-MnS/Ti_(3)C_(2)T_(x))composite material derived from Mn-based metal-organic framework is *** tests show that Se-doped could generate S defects and enhance the electrochemical activity of *** the same time,the introduction of Ti_(3)C_(2)T_(x) substrate is conducive to exposing more sulfur defects and improving the utilization rate of *** the mechanism study,it is found that Se-MnS/Ti_(3)C_(2)T_(x) is transformed into S/Se co-doped Mn3O_(4) at the first charge,which innovatively elucidated the behavior of S/Se during *** the electrochemical performance test,the specific capacity can reach 74.7 mAh·g^(-1) at 5.0 A·g^(-1).In addition,the Zn-Ti_(3)C_(2)T_(x) membrane electrode is prepared by vacuum filtration as the zinc-poor anode,which is assembled into the rocking chair full battery to avoid dendrite growth and exhibit excellent rate *** addition of Zn2+weakens the electrostatic repulsion between the interlayers of MXene,and the formation of the folded morphology aids the penetration of the *** 1.0 A·g^(-1),the capacity can reach 50.6 mAh·g^(-1).This work is helpful to promote the research and development of the reaction mechanism of manganese based rocking chair batteries.

关键词： rocking-chair zinc-ion battery MnS Zn-Ti_(3)C_(2)T_(x) membrane Se doped Ti_(3)C_(2)T_(x) composite

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In situ protonation in a locally flexible porous coordination polymer for enhancing proton-carrier loading and proton conductivity

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Science China chemistry 2024年第10期67卷 3432-3437页

作者： Xianzhe Wei Jincheng Liu Yan Su Weitao Wang Guixiang Wang Gen Zhang Ping Wang Cheng Gu State Key laboratory of Luminescent materials and Devices Institute of Polymer Optoelectronic Materials and DevicesSouth China University of TechnologyGuangzhou 510640China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China Key laboratory for Soft chemistry and Functional materials of Ministry of Education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing 210094China

Designing efficient proton-conductive materials is crucial in fuel ***,it remains a substantial challenge because of the issues in proton mobility,proton-carrier amount,and orientation of proton host ***,we report an in-situ protonation strategy to produce a locally flexible porous coordination polymer(PCP)to enhance the proton-carrier loading and proton *** local dipole flipping of the ligand allows effective proton exchange with low activation energy,promoting interpore proton transport through the pore apertures and pore *** protonation induces substantial charges to the frameworks and enhances the interaction with proton carriers,thereby increasing the loading of the proton *** this design strategy,the resulting PCP exhibits enhanced phosphoric acid loading and extraordinary proton conductivities under both aqueous and anhydrous conditions compared to its isoreticular analog that features rigidity without proton-exchange *** work provides a new avenue for designing proton-conductive materials that combine structural dynamics with performance merits.

关键词： porous coordination polymers in-situ protonation local flexibility proton-exchange mechanism proton conduction

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Furfural residues derived nitrogen-sulfur co-doped sheet-like carbon: An excellent electrode for dual carbon lithium-ion capacitors

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Green Energy & Environment 2024年第9期9卷 1427-1439页

作者： Xiaoying Guo Yan Qiao Zonglin Yi Christian Marcus Pedersen Yingxiong Wang Xiaodong Tian Peide Han College of materials Science and Engineering Taiyuan University of Technology State Key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences CAS Key laboratory of Carbon materials Institute of Coal Chemistry Chinese Academy of Sciences Department of chemistry University of Copenhagen Universitetsparken 5 College of chemistry Taiyuan University of Technology

The state-of-the-art lithium-ion capacitors （LICs）,consisting of high-capacity battery-type anode and high-rate capacitor-type cathode,can deliver high energy density and large power density when comparing with traditional supercapacitors and lithium-ion batteries,***,the ion kinetics mismatch between cathode and anode leads to unsatisfied cycling lifetime and anode *** efforts have been devoted to solving the abovementioned *** promising strategy is altering high conductive hard carbon anode with excellent structural stability to match with activated carbon cathode,assembling dual-carbon *** this contribution,one-pot in-situ expansion and heteroatom doping strategy was adopted to prepare sheet-like hard carbon,while activated carbon was obtained involving *** persulfate was used as expanding and doping agent *** furfural residues （FR） were served as carbon *** resulting hard carbon （FRNS-HC） and activated carbon （FRNS-AC）show excellent electrochemical performance as negative and positive electrodes in a lithium-ion battery （LIB）.To be specific,374.2 m Ah g-1and 123.1 m Ah g-1can be achieved at 0.1 A g-1and 5 A g-1when FRNS-HC was tested as *** combined with a highly porous carbon cathode (SBET=2961 m2g-1) synthesized from the same precursor,the LIC showed high specific energy of147.67 Wh kg-1at approximately 199.93 W kg-1,and outstanding cycling life with negligible capacitance fading over 1000 *** study could lead the way for the development of heteroatom-doped porous carbon nanomaterials applied to Li-based energy storage applications.

关键词： Furfural residue Ammonium persulfate Sheet-like carbon Lithium-ion capacitors Hard carbon

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Increase of chiral sensing ability in host-guest chemistry by magnetic anisotropy

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Science China chemistry 2024年第8期67卷 2775-2782页

作者： Jia-Liang Chen Bin Li Feng Yang Tiesheng Shi Xun-Cheng Su State Key laboratory of Elemento-organic chemistry Tianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China College of chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160China

Enantiomeric molecules generally play distinct functions in chemistry,biology,and *** physical and chemical properties of chiral analytes lay difficulty in discrimination and quantification of the *** report herein an efficient approach of increasing the chiral sensing ability ofβ-cyclodextrin(β-CD),a widely used host molecule,in the hostguest chemistry by magnetic anisotropy.A rigid and chiral lanthanide binding tag was attached to theβ-CD to amplify the changes of nuclear magnetic resonance(NMR)signals in the host-guest recognition *** installation of the paramagnetic lanthanide ion inβ-CD greatly enhances the enantiomeric discrimination up to 30-fold in comparison with the diamagneticβ-CD *** addition,the magnitude of the paramagnetic effects is tunable according to the diverse range of paramagnetic strength of the lanthanide *** reported method significantly increases the chiral sensing ability ofβ-CD,which can be applied to other host *** transferred paramagnetic effects,pseudocontact shifts(PCSs)and paramagnetic relaxation enhancements(PREs),from the host to the guest molecules,are valuable structural restraints to determine the absolute stereochemistry of the chiral *** strategy does not need modification of the analytes and is complementary to the reported analytical methods that rely on the functionalization of the chiral analytes.

关键词： chiral recognition nuclear magnetic resonance host-guest chemistry magnetic anisotropy lanthanide ions

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Acylfluorination of enynes via phosphine and silver catalysis

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Chinese Chemical Letters 2024年第8期35卷 260-264页

作者： Yu Mao Yilin Liu Xiaochen Wang Shengyang Ni Yi Pan Yi Wang State Key laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

This work describes intermolecular acylfluorination of gem-difluoroenynes using acyl fluorides as both acyl source and fluorine ***-substituted allenones or furans could be selectively achieved via phosphine and silve... 详细信息

关键词： Phosphine catalysis Silver catalysis Difunctionalization Allenone Furan Trifluoromethyl

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