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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

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 ***, 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

Crafting host materials for narrowband blue OLEDs with low efficiency roll-off by the medium-ring strategy

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Science China chemistry 2024年第10期67卷 3265-3270页

作者： Yuanyuan Bao Anping Luo Jingbo Lan Junjie Liu Zhengyang Bin Jingsong You key laboratory of Green chemistry and Technology of ministry of education College of ChemistrySichuan University

The pursuit of high-performance narrowband blue organic light-emitting diodes（OLEDs） is of paramount importance in both academic research and industrial *** obvious strides have been made in the design of narrowband blue emitters,the development of appropriate host materials has evidently trailed ***,we introduce a medium-ring strategy for crafting host molecules based on the heptagonal tribenzo[b,d,f]azepine（TBA） *** twisted three-dimensional（3D） architecture of the TBA framework not only endows the host molecules with fast hole-transporting pathways but also effectively reduces exciton *** with two TBA units,DTBA,synthesized with ease,demonstrates a huge horizontal orientation factor(Θ//) of 93.5%and a broad emission spectrum for accelerating the energy transfer process in the emitting layer,which contributes to enhancing device *** have fabricated high-performance narrowband blue OLEDs using DTBA as the host,FIrpic as the phosphor sensitizer,and the widely used boron-nitrogen-containing multiple resonance emitter *** devices exhibit a maximum external quantum efficiency(EQEmax) as high as 31.0% with an impressively lowefficiency *** at a high luminance level of 10,000 cd m-2,the EQE value remains noteworthy at 20.3%,marking a significant advancement in BCz-BN-based devices.

关键词： host molecule blue organic light-emitting diode low-efficiency roll-off multiple resonance C–H activation

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Syntheses of new di-nuclear and tetra-nuclear lanthanide 9-anthracenecarboxylates:Magnetocaloric effect,slow magnetic relaxation and luminescent properties

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Journal of Rare Earths 2024年第6期42卷 1101-1109,I0004页

作者： Xing Liu Ruonan Yang Lu Zhang Jian Zhou Chunmei Huang Huahong Zou Zunhong Xiao Chongqing key laboratory of Inorganic functional Materials College of ChemistryChongqing Normal UniversityChongqing401331China key laboratory for the chemistry and molecular Engineering of Medicinal Resources(ministry of education of China) School of Chemistry and Chemical Engineering of Guangxi Normal UniversityGuilin541004China School of chemistry and Materials Guizhou Normal UniversityGuiyang550025China

Lanthanide complex-based materials with magnetic and luminescent properties have received a great deal of attention,owing to their importantly potential applications in diverse *** this work,the 9-anthracenecarboxylic acid(9-Haca)as bridging ligand was applied in combination with optically activeπ-conjugated 2,4,6-tri(2-pyridyl)-1,3,5-triazine(tptz)to construct a series of new di-nuclear and tetranuclear lanthanide 9-anthracenecarboxylates[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]·0.25H_(2)O(1),[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]·0.5AQ·CH_(3)COOH_(2)H_(2)O[Ln=Sm(2a),Eu(2b),Gd(2c),Tb(2d),Dy(2e),Tm(2f);AQ=9,10-anthracenedione]and[Ln_(4)(9-aca)_(10)(tptz)_(2)(CH3COO)2]·H_(2)O[Ln=Eu(3a),Gd(3b),Dy(3c)].1 displays a di-nuclear centrosymmetric moiety[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]built up from two complex[La(9-aca)_(2)(tptz)]groups bridged by one H_(2)O molecule and two syn-syn-μ2-η1:η1-9-aca-bridging ligands,while 2a-2f are isostructural and co mprise another di-nuclear centrosymmetric moieties[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]based on two complex[Ln(9-aca)_(2)(tptz)(H_(2)O)]groups connected by two syn-syn-μ2-η1:η1-9-aca-bridging ligands,3a-3c are isostructural and show tetra-nuclear centro symmetric moieties[Ln4(9-aca)10(tptz)2(CH3COO)2]containing three types of coordination modes of *** present compounds offer the only examples of lanthanide 9-anthracenecarboxylates decorated by optically active *** investigations of 2a,2c-2f,and 3b-3c indicate that 3c is typical of slow relaxation of the magnetization,while 2c and 3b show significant magnetocaloric effect(MCE)with the value of-ΔSm of 5.26 J/(kg·K)at 4 K and 15.65 J/(kg·K)at 2 K(ΔH=7 T),*** luminescent properties were also studied and reveal that the characteristic luminescent properties of the 7r-conjugated aromatic ligands are introduced into magnetic lanthanide 9-anthracenecarboxylates,simultaneously exhibiting slow magnetic relaxation(or MCE)and luminescen

关键词： Lanthanide complexes Luminescence Magnetic properties Magnetocaloric effect Slow magnetic relaxation Rare earths

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

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 *** 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 ***,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 *** 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 *** 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

Progress of photocatalytic COreduction toward multi-carbon products

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Science China chemistry 2024年

作者： Jiaojiao Fang Chengyang Zhu Huiling Hu Jiaqi Li Licheng Li Haiyan Zhu Junjie Mao key laboratory of functional molecular Solids Ministry of Education College of Chemistry and Materials ScienceAnhui Normal University

The photocatalytic CO2reduction reaction （CO2RR） represents a promising solution to alleviate environmental and energy issues stemming from CO2emissions while simultaneously enabling the production of high-value multi-carbon ***,the efficient generation of multi-carbon products remains challenging due to high kinetic barriers,sluggish C–C coupling processes,and intricate reaction *** review provides a comprehensive overview of the latest advancements in synthesizing C2+products through CO2photoreduction,highlighting the crucial role of active site design and the C–C coupling ***,we emphasize the correlation between the structure of active sites and the key intermediates of C–C coupling,which is fundamental for achieving deep photoconversion of ***,we offer a glimpse into future challenges and prospects,outlining potential directions for the development of CO2-to-multicarbon photoconversion,aiming to contribute novel insights to this exciting field.

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Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia: highly active catalysts for n-hexane combustion

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Green Energy & Environment 2024年第7期9卷 1122-1137页

作者： Xiuqing Hao Yuxi Liu Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai Beijing key laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution Control Key Laboratory of Advanced Functional Materials Education Ministry of China Laboratory of Catalysis Chemistry and Nanoscience Department of Chemical Engineering Faculty of Environment and Life Beijing University of Technology

Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds （VOCs）.In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom （Co1Ni1/meso-Cr2O3） and bimetallic Co and Ni nanoparticle (CoNPNiNP/mesoCr2O3) catalysts adopting the one-pot polyvinyl pyrrolidone （PVP）-and polyvinyl alcohol （PVA）-protecting approaches,*** results indicate that the Co1Ni1/meso-Cr2O3catalyst exhibited the best catalytic activity for n-hexane (C6H14) combustion (T50%and T90%were 239 and 263℃ at a space velocity of 40,000 mL g-1h-1;apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol-1and 4.3×10-7mol g-1cats-1,respectively),which was associated with its higher (Cr5++Cr6+) amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni1was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co1preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen（MvK） mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→COx→CO2and H2O.

关键词： Three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt−nickel single atoms n -Hexane combustion Catalytic reaction mechanism

Photoinduced generation of alkyl and phthalimide nitrogen radicals from N-hydroxyphthalimide esters for the synthesis of benzophenone-type bioisosteres

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Science China chemistry 2024年第10期67卷 3389-3396页

作者： Fei Li Jianyang Dong Huijuan Liao Jiayi Dang Xuechen Zhou Yuying Wang Chenya Wang Qin Jiang Gang Li Dong Xue key laboratory of Applied Surface and Colloid chemistry Ministry of Education and School of Chemistry and Chemical EngineeringShaanxi Normal University

N-Hydroxyphthalimide（NHPI） esters have emerged as powerful sources of alkyl radicals generated by single-electron transfer,but homolysis of NHPI ester to produce an alkyl radical and a phthalimide nitrogen radical is still in its infancy. In this study, we developed a light-induced method for generation of alkyl and phthalimide nitrogen radicals from NHPI esters and subsequent reactions of the radicals with [1.1.1]propellane and aryl aldehydes for rapid generation of bicycle [1.1.1]pentane ketones. This method does not require metals or photosensitizers, features a broad substrate scope（90 examples） and excellent functional group tolerance, and can be used for the functionalization of structurally complex natural products and drugs. Mechanistic investigations indicate that the reaction involves photoinduced homolytic cleavage of the Cs2CO3-NHPI ester complex to produce alkyl and phthalimide nitrogen radicals and subsequent hydrogen atom transfer between the phthalimide nitrogen radical and the aldehyde to generate an acyl radical.

关键词： phthalimide nitrogen radicals aryl aldehydes hydrogen atom transfer bicycle[1.1.1]pentane ketones bioisosteres