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Azocalixarenes: a scaffold of universal excipients with high efficiency

Science China chemistry 2024年第5期67卷 1697-1706页

作者： Yu-Xin Yue Yi-Lin Lin Meng-Meng Chen Han-Wen Tian Rong Ma Ze-Han Wang Fang-Yuan Chen Yu-Chen Pan Dong-Sheng Guo College of chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Functional Polymer Materials(Ministry of Education)Frontiers Science Center for New Organic MatterCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin 300071China

Excipients are important components of pharmaceutical preparations that affect their quality, safety, and efficacy. Macrocyclic receptors are a family of supramolecular excipients with several advantages, including molecular-level protection, small sizes,fast kinetics of host-guest recognition, and modular construction. With the continuous advances in the medical field, personalized and precision medicine requires the development of excipients with low dosages, integrated modifying effects, universality,and controlled release. To meet these requirements, we have developed a new family of macrocyclic excipients based on calixarenes by integrating their covalent(broad chemical design space) and noncovalent(wide range of substrates) ***, azocalixarenes(Azo CAs) were designed, showing high binding affinities to a broad spectrum of active pharmaceutical ingredients(APIs), selectivity to interferents, and responsiveness to hypoxic microenvironments. Due to their highly efficient and controllable recognition, Azo CAs serve as low-dose excipients for 30 APIs. Molecular encapsulation by Azo CAs results in the integrated modification of the physicochemical properties of APIs, including solubility, stability, bioavailability,and biocompatibility. Moreover, Azo CAs can be reduced by azoreductases overexpressed in hypoxic microenvironments,leading to the controlled release of APIs. Collectively, Azo CA excipients have broad application prospects for a series of diseases such as enteritis, arthritis, stroke, cancer, bacterial infection and kidney injury, with diverse therapeutic modalities,including chemotherapy, photodynamic therapy, photothermal therapy, immunotherapy, boron neutron capture therapy, radiotherapy, fluorescence imaging, and their combinations.

关键词： supramolecular chemistry host-guest systems excipient calixarene molecular recognition

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Precise phase adjustment and antibacterial property of copper sulfide particles in confined mesoporous silica nanoreactor

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Particuology 2024年第2期85卷 113-121页

作者： Shiyu Xu Jinyong Wu Zhongzhen Ren Dechao Niu Low Dimensional Materials chemistry laboratory Key Laboratory for Ultrafine Materials of Ministry of EducationFrontier Science Center of the Materials Biology and Dynamic ChemistryShanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China

Bacteria-caused wound infection greatly threatens human health,thus developing an efficient and safe antibacterial agent without drug resistance is still a great ***,a confined vulcanization strategy is proposed to construct copper sulfides-loaded dual-mesoporous silica nanospheres(Cux-Sy@DMSNs)with various crystal phases for reactive oxygen species(ROS)-mediated and photothermal antibacterial *** the pore confinement of DMSNs,the crystal phases of copper sulfides including CuS,Cu_(9)S_(5)and Cui.96S can be easily controlled by changing the vulcanization *** relationships between the crystal phases and photothermal properties as well as peroxidase-like activity of copper sulfides were systematically *** show that the obtained CuS@DMSNs exhibited higher photothermal ability with remarkable photothermal conversion efficiency of 36.86%in the second near-infrared region(NIR-II)and better peroxidase-like activity,compared to those of Cu_(9)S_(5)@DMSNs and Cu_(1.96)S@*** a result,the in vitro experiments showed the good antibacterial effect against both gram-negative *** and gram-positive *** under 1064 nm laser irradiation and the presence of H_(2)O_(2).Besides,the CCK-8 assay indicated that CuS@p-DMSNs have minimal cytotoxicity against normal human umbilical vein endothelial cells at the ranged ***,the resultant CuS@p-DMSNs could act as a promising antibacterial agent for deep wound bacterial infection treatment.

关键词： Copper sulfides Mesoporous silica Photothermal Reactive oxygen species Antibacterial agent

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Unique Azolyl Acylhydrazonyl Hybridization of Aloe Emodins to Access Potential Antibacterial Agents

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Chinese Journal of chemistry 2024年第15期42卷 1741-1758页

作者： Yi-Xin Wang Zhao Deng Aisha Bibi Bo Fang Cheng-He Zhou Institute of Bioorganic&Medicinal chemistry Key Laboratory of Applied Chemistry of Chongqing MunicipalitySchool of Chemistry and Chemical EngineeringSouthwest UniversityChongqing 400715China College of Pharmacy National&Local Joint Engineering Research Center of Targeted and Innovative TherapeuticsChongqing Key Laboratory of Kinase Modulators as Innovative MedicineChongqing University of Arts and SciencesChongqing 402160China

A type of unique azole-hybridized acylhydrazonyl aloe emodins(AAEs)were developed as new antibacterial agents for combating bacterial *** target AAEs showed strong antibacterial activities,especially,tetrazolylthioether AAE 27a exhibited broad antibacterial spectrum with 16-256 folds and 8-64 folds more active antibacterial efficacy than the reference drugs aloe emodin and norfloxacin,*** AAE 27a also gave low hemolysis and cytotoxicity,as well as favorable *** mechanism explorations revealed that tetrazolylthioether AAE 27a could cause bacterial membrane depolarization and damage the cell membrane,resulting in nucleic acid ***,compound 27a could intercalate into DNA to impede its replication and form supramolecular 27a-DNA gyrase complex to disturb the function of DNA *** findings would provide valuable insights for the further exploration of azolyl acylhydrazonyl aloe emodins as new potential antibacterial candidates.

关键词： Aloe emodin Hydrazone Heterocycle Antibacterial Membrane damage

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Ultrastable graphene isolated Au Ag nanoalloy for SERS biosensing and photothermal therapy of bacterial infection

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Chinese Chemical Letters 2024年第3期35卷 198-203页

作者： Shengkai Li Zhiyang Li Qing Hao Shen Wang Yanxia Yang Jieqiong Xu Zhiwei Yin Liang Zhang Zhuo Chen Molecular Science and Biomedicine laboratory(MBL) State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollege of BiologyAptamer Engineering Center of Hunan ProvinceHunan UniversityChangsha 410082China School of chemistry and Chemical Engineering/Guangzhou Key laboratory for Clean Energy and Materials/Key laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationGuangzhou UniversityGuangzhou 510006China

Plasmonic metal nanomaterials with intrinsic surface–enhanced Raman scattering(SERS)and photothermal properties,especially AuAg nanoalloys with both the outstanding merits of Au and Ag nanocrystals,show huge application prospects in bacterial ***,the direct exposure of AuAg nanoalloys in external conditions probably cause undesirable reactions and poisonous metal ion leakage during SERS detection and photothermal antibacterial therapy process,which severely hinder bacterial theranostics ***,we report an ultrastable graphene–isolated AuAg nanoalloy(GAA)with AuAg core confined in few–layer graphitic shell as a versatile platform for bacterial detection and *** encapsulation of graphene ensures the good stability of AuAg core,that its superior SERS and photothermal properties are therefore further *** is used for SERS detection of two vital bacterial biomarkers(including corrosive cyanide and pyocyanin),exhibiting good SERS quantitative and multiplexing *** is further used for photothermal antibacterial therapy application,and ultrahigh antibacterial efficacies for both Gram–negative Escherichia coli and Gram–positive Staphylococcus aureus are achieved under 808 nm laser *** work proposes a valuable method to develop robust bacterial theranostic platform.

关键词： Localized surface plasmon resonance Graphitic shell isolated AuAg nanoalloy(GAA) Surface–enhanced Raman scattering(SERS) bacterial biomarker detection Photothermal antibacterial therapy

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Bioinspired polysaccharide-based nanocomposite membranes with robust wet mechanical properties for guided bone regeneration

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National Science Review 2024年第3期11卷 215-226页

作者： Jian-Hong Xiao Zhen-Bang Zhang JiaHao Li Si-Ming Chen Huai-Ling Gao YinXiu Liao Lu Chen ZiShuo Wang YiFan Lu YuanZhen Hou HengAn Wu DuoHong Zou Shu-Hong Yu Department of chemistry New Cornerstone Science Laboratory Institute of Biomimetic Materials&Chemistry Anhui Engineering Laboratory of Biomimetic MaterialsDivision of Nanomaterials&Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Department of Dental Implant Center Stomatologic Hospital and College Key Laboratory of Oral Diseases Research of Anhui Province Anhui Medical University CAS Key laboratory of Mechanical Behavior and Design of Materials Department of Modern Mechanics CAS Center for Excellence in Complex System Mechanics University of Science and Technology of China Department of Oral Surgery College of Stomatology National Clinical Research Center for Oral DiseasesShanghai Key Laboratory of Stomatology Shanghai Research Institute of Stomatology Shanghai Ninth People's Hospital Affiliated to Shanghai Jiao Tong University School of Medicine Institute of Innovative Materials(I2M) Department of Chemistry Department of Materials Science and Engineering Southern University of Science and Technology

Polysaccharide-based membranes with excellent mechanical properties are highly desired. However, severe mechanical deterioration under wet conditions limits their biomedical applications. Here, inspired by the structural heterogeneity of strong yet hydrated biological materials, we propose a strategy based on heterogeneous crosslink-and-hydration（HCH） of a molecule/nano dual-scale network to fabricate polysaccharide-based nanocomposites with robust wet mechanical properties. The heterogeneity lies in that the crosslink-and-hydration occurs in the molecule-network while the stress-bearing nanofiber-network remains unaffected. As one demonstration, a membrane assembled by bacterial cellulose nanofiber-network and Ca2+-crosslinked and hydrated sodium alginate molecule-network is designed. Studies show that the crosslinked-and-hydrated molecule-network restricts water invasion and boosts stress transfer of the nanofiber-network by serving as interfibrous bridge. Overall, the molecule-network makes the membrane hydrated and flexible; the nanofiber-network as stress-bearing component provides strength and *** HCH dual-scale network featuring a cooperative effect stimulates the design of advanced biomaterials applied under wet conditions such as guided bone regeneration membranes.

关键词： bioinspiration heterogeneous crosslink-and-hydration dual-scale network nanocomposite membrane wet mechanical properties guided bone regeneration

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Triclosan-conjugated,Lipase-responsive Polymeric Micelles for Eradication of Staphylococcal Biofilms

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Chinese Journal of Polymer Science 2024年第6期42卷 718-728页

作者： Yan-Qiang Huang Yuan-Feng Li Yong Liu Lin-Qi Shi Guangxi Technology Innovation Cooperation Base of Prevention and Control Pathogenic Microbes with Drug Resistance Youjiang Medical University for NationalitiesBaise533000China Translational Medicine laboratory the First Affiliated Hospital of Wenzhou Medical UniversityWenzhou325035China Wenzhou Institute University of Chinese Academy of SciencesWenzhou325001China State Key laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials of Ministry of Educationand Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin300071China

bacterial biofilms present a significant challenge in treating drug-resistant infections,necessitating the development of innovative *** this study,we introduce triclosan-conjugated,lipase-responsive polymeric micelles designed to exploit biofilm properties and serve as a responsive drug delivery *** micelles were created using an amphiphilic block polymer synthesized via ring-opening polymerization ofε-caprolactone(CL)and triclosan-containing cyclic trimethylene carbonate(MTC-Tri).Poly(ethylene glycol)(PEG-OH)acted as the macro-initiator,resulting in micelles with a PEG shell that facilitated their penetration into bacterial *** important advantage of our micelles lies in their interaction with local bacterial lipases within *** lipases triggered rapid micelle degradation,releasing triclosan in a controlled *** liberated triclosan effectively eliminated bacteria embedded in the ***,the triclosan-conjugated micelles displayed minimal toxicity to murine fibroblasts,indicating their biocompatibility and *** finding emphasizes the potential application of these micelles in combatting drug resistance observed in bacterial *** triclosan-conjugated,lipase-responsive polymeric micelles exhibit promising characteristics for addressing drug resistance in bacterial *** harnessing biofilm properties and implementing a responsive drug delivery system,we seek to provide an effective solution in the fight against drug-resistant bacteria.

关键词： Self-assembly Polymer prodrug Ring-opening polymerization Biofilm eradication Cytotoxicity

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A Degradable Quaternary Ammonium-Based Pesticide Safe for Humans

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CCS chemistry 2024年第6期6卷 1499-1511页

作者： Wenwen Han Xiao-Qi Xu Xiaodong Lian Yanji Chu Yapei Wang Key laboratory of Advanced Light Conversion Materials and Biophotonics Department of ChemistryRenmin University of ChinaBeijing 100872

Reducing the emission of agrochemicals hazardous to the environment and human health is one of the key targets of the UN’s Sustainable Development Goal ***,we report a kind of quaternary ammonium pesticides with an acid-cleavable silaketal linkage on their backbones that enables control of *** pesticides possess outstanding bactericidal and insecticidal properties but become harmless to humans and other organisms after *** on the conditions of use,the hydrolytic process can be controlled over the time range of 10 min to 3 *** laboratory simulations and agricultural field demonstrations confirm that these pesticides can effectively protect crops from bacterial diseases and *** the sametime,single-dose intragastric administration using diisopropylsilyloxy bisquaternary ammonium salt 9(ISBQAS-9)in mice demonstrates its safety for multiple *** to the advantages of controllable degradability,environmental friendliness,and the low financial cost of these pesticides,this welldesigned strategy holds great promise for the generation of environmentally harmless pesticides and the development of green agriculture.

关键词： antimicrobial materials degradable pesticides insecticidal materials quaternary ammonium surfactants stimulus-cleavable chemistry

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A noval iron-capturing nanocomposites against biofilms for disrupting bacterial nutritional balance

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Science China chemistry 2024年第6期67卷 1760-1761页

作者： Jinying Lin Qihang Ding Yao Sun Department of Oral Implantology Jilin Provincial Key Laboratory of Tooth Development and Bone RemodelingSchool of StomatologyJilin UniversityChangchun130021China Department of chemistry Korea UniversitySeoul02841Korea National Key laboratory of Green Pesticide International Joint Research Center for Intelligent Biosensor Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan430079China

Currently,the escalating crisis of bacterial infections and antibiotic resistance poses a significant global public health challenge[1-3].This situation has driven the search for novel antimicrobial ***,a crucial micr... 详细信息

关键词： metabolism resistance balance

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Construction of algal-bacterial consortia using green microalgae Chlorella vulgaris and As(Ⅲ)-oxidizing bacteria:As tolerance and metabolomic profiling

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Journal of Environmental Sciences 2024年第5期139卷 258-266页

作者： Xiaoman He Guobing Lin Jiayuan Zeng Zhaoguang Yang Lin Wang College of chemistry and Chemical Engineering Central South UniversityChangsha 410083China Key laboratory of Hunan Province for Water Environment and Agriculture Product Safety Central South UniversityChangsha 410083China

Bioremediation became a promising technology to resolve arsenic(As)contamination in aquatic *** monoculture such as microalgae or bacteria was sensitive to environmental disturbance and vulnerable to contamination,green microalgae Chlorella vulgaris and arsenite(As(Ⅲ))-oxidizing bacteria Pseudomonas ***11 were co-cultured to construct algal-bacterial consortia in the current *** effects of algae-bacteria(A:B)ratio and exposure As(Ⅲ)concentration on algal growth,As speciation and metabolomic profile were *** growth arrested when treated with 100 mg/L As(Ⅲ)without the co-cultured *** contrast,co-cultured with strain SMS11 significantly enhanced As tolerance in *** especially with A:B ratio of 1:*** the As(Ⅲ)in culture media of the consortia were oxidized into As(Ⅴ)on day *** of As was observed on day *** 1% and 0.5% of total As were converted into dimethylarsinic acid(DMA)after 21days cultivation when the initial concentrations of As(Ⅲ)were 1 and 10 mg/L,*** analysis was further performed to reveal the response of consortia metabolites to external As(Ⅲ).The enriched metabolomic pathways were associated with carbohydrate,amino acid and energy *** acid cycle and glyoxylate and dicarboxylate metabolism were upregulated under As stress due to their biological functions on alleviating oxidative stress and protecting *** carbohydrate and amino acid metabolisms provided precursors and potential substrates for energy production and cell protection under abiotic *** of the pathways relevant to carbohydrate or amino acid metabolism were triggered by energy requirement.

关键词： Microalgae Algal-bacterial consortia As(Ⅲ)-oxidizing bacteria Metabolomics Energy metabolism

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Dynamic shielding of bacterial outer membrane vesicles for safe and efficient chemo-immunotherapy against tumors

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Nano Research 2024年第2期17卷 836-847页

作者： Shuping Li Xin Li Jiaqi Meng Weier Bao Shuang Wang Peng Ye Xiao-Dong Gao Wei Wei Key laboratory of Carbohydrate chemistry and Biotechnology Ministry of Education School of BiotechnologyJiangnan UniversityWuxi 214122China State Key laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

bacterial outer membrane vesicles(OMVs)are potent immunostimulants of regulating the tumor microenvironment(TME)for immunotherapy,and can be used to deliver ***,the severe systemic inflammatory response triggered by OMVs upon intravenous(i.v.)injection has limited their ***,we developed a safe and effective strategy by conjugating doxorubicin-loaded serum albumin(SA-DOX,AD)onto the surface of OMVs using a matrix metalloproteinase(MMP)-cleavable peptide linker(cL).This approach enabled the dynamic shielding of OMVs to reduce the systemic side effects while simultaneously enhancing the anti-tumor effects through ***,the resulting OMV-cL-AD formulation exhibited significantly enhanced accumulation at the tumor site after ***,facilitated by the SA decoration on the OMVs ***,the shield on the OMV-cL-AD was cleaved by the over-expressed MMP in the TME,leading to the release of both OMVs and *** process provided OMV-induced immunotherapy and DOX-induced chemotherapy,resulting in synergistic tumor *** conclusion,our work demonstrated the potential of OMV-cL-AD as an effective immunochemotherapy strategy that can prolong the survival time of mice without inducing side effects.

关键词： outer membrane vesicles doxorubicin tumor microenvironment immunotherapy chemotherapy

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