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Science China Chemistry 2024年第6期67卷 1881-1903页

作者： Dayang Wang Xiaohua Li Huanchen Yao Xin Liu Yan Gao Hailin Cong Bing Yu Youqing Shen College of Chemistry and Chemical Engineering College of Life SciencesCollege of Materials Science and EngineeringInstitute of Biomedical Materials and EngineeringQingdao UniversityQingdao266071China State Key Laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdao266071China School of Materials Science and Engineering Shandong University of TechnologyZibo255000China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Center for Bionanoengineeringand Department of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China

Nanomedicine delivery technology plays an important role in modern medicine and has shown good therapeutic effects in scientific research.Polysaccharides have the characteristics of wide sources,excellent biocompatibility,and non-toxicity.In addition,there are multifunctional groups on the main chain of polysaccharides,which can be surface-modified or functionalized to have targeting ability through specific sugar parts.Amphiphilic polysaccharide micelles with good biocompatibility,degradability,high safety,easy structural modification,and special core-shell structure are regarded as ideal carriers for nanomedicines.Therefore,this review is focused on the hydrophobic modification designs of polysaccharides,the preparation methods and characteristics of micelles,and the applications of amphiphilic polysaccharide micelles in the field of biomedicine.It is expected to provide some ideas and inspiration for the design of polysaccharide drug carriers.

关键词： polysaccharide hydrophobic modification micelle drug delivery biomedicine

In Situ Sustained Macrophage-Targeted Nanomicelle-Hydrogel Microspheres for Inhibiting Osteoarthritis

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Research 2024年第1期2023卷 1-16页

作者： XiaoXiao Li Xingchen Li Jielai Yang Yawei Du Liang Chen Gang Zhao Tingjun Ye Yuan Zhu Xiangyang Xu Lianfu Deng Wenguo Cui Department of Orthopaedics Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint DiseasesShanghai Institute of Traumatology and OrthopaedicsRuijin HospitalShanghai Jiao Tong University School of MedicineShanghai 200025P.R.China

There are stillchallenges in applying drug nanocarriers for in situ sustained macrophage targeting and regulation,due to the rapid clearance of nanocarriers and burst drug release invivo.Herein,a nanomicellehydrogel microsphere,characterized by its macrophage-targeted nanosized secondary structure that allows it to accurately bind to M1 macrophages through active endocytosis,is employed for in situ sustained macrophage targeting and regulation,and addresses the insufficient osteoarthritis therapeutic efficacy caused by rapid clearance of drug nanocarriers.The 3-dimensional structure of a microsphere can prevent the rapid escape and clearance of a nanomicelle,thus keeping it in joints,while the ligand-guided secondary structure can carry drugs to accurately target and enter M1 macrophages,and release drugs via the transition from hydrophobicity to hydrophilicity of nanomicelles under inflammatory stimulation inside the macrophages.

关键词： micelle release spheres

Intracellular and extracellular enzymatic responsive micelle for intelligent therapy of cancer

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Nano Research 2023年第2期16卷 2851-2858页

作者： Dong Wan Qinan Zhu Jianxin Zhang Xi Chen Fangzhou Li Yi Liu Jie Pan School of Chemical Engineering and Technology Tiangong UniversityTianjin 300387China School of Chemistry Tiangong UniversityTianjin 300387China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China

Recently,the incidence of cancer keeps increasing,seriously endangers human health,and has evolved into the main culprit of human death.Conventional chemotherapeutic drugs,such as paclitaxel and doxorubicin(DOX),have some disadvantages,including low therapeutic effect,poor water solubility,high toxic side effects,short blood circulation time in the body,and so on.To improve the anti-tumor effect of the drug in vivo and reduce its side effects on the body,researchers have designed and developed a variety of responsive nanocarriers.In this work,we synthesized D-α-tocopherol polyethylene glycol 3350 succinate(TPGS3350)-Gly-Pro-Leu-Gly-Val-Arg(GPLGVR)-DOX(TPD)prodrugs in response to extracellular enzymes of matrix metalloproteinase(MMP-9)in the tumor microenvironment and FA-Asp-Glu-Val-Asp(DEVD)-DOX(FPD)prodrugs responsive to intracellular enzymes of caspase-3.Then,intracellular and extracellular enzyme-responsive TPD&FPD micelles with DOX(TPD&FPD&D)were successfully prepared through dialysis method.The outer layer of TPGS3350 can prolong the blood circulation time of micelles in vivo,followed by accumulation of micelles at tumor tissue through enhanced permeability and retention(EPR)effect.The peptide of GPLGVR can be cleaved by MMP-9 enzymes to remove the outer layer of TPGS3350,exposing the targeting molecule of folate,and then the micelles are engulfed by tumor cells through folate receptor-mediated endocytosis.After entering the tumor cells,the free DOX loaded in the micelles is released,which induces tumor cell apoptosis to activate caspase-3 in the cells,cutting the peptide DEVD to accelerate the intracellular release of the DOX,which further enhances cytotoxicity to improve antitumor effect.

关键词： cancer micelle peptide enzyme-responsive folate

Delivery of coenzyme Q10 loaded micelle targets mitochondrial ROS and enhances efficiency of mesenchymal stem cell therapy in intervertebral disc degeneration

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Bioactive Materials 2023年第5期23卷 247-260页

作者： Junyuan Sun Fei Yang Lianlei Wang Haichao Yu Zhijie Yang Jingjing Wei Krasimir Vasilev Xuesong Zhang Xinyu Liu Yunpeng Zhao Department of Orthopaedics Qilu HospitalCheeloo College of MedicineShandong UniversityJinanShandong250012PR China School of Pharmaceutical Sciences Shandong UniversityJinanShandong250012PR China School of Medicine Nankai UniversityTianjin300071PR China Department of Orthopaedics The Fourth Medical CentreChinese People’s Liberation Army General HospitalBeijing100048PR China Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinanShandong250100PR China Academic Unit of STEM University of South AustraliaMawson LakesAdelaide5095South AustraliaAustralia College of Medicine and Public Health Flinders UniversityBedford Park5042South AustraliaAustralia

Stem cell transplantation has been proved a promising therapeutic instrument in intervertebral disc degeneration(IVDD).However,the elevation of oxidative stress in the degenerated region impairs the efficiency of mesenchymal stem cells(BMSCs)transplantation treatment via exaggeration of mitochondrial ROS and promotion of BMSCs apoptosis.Herein,we applied an emulsion-confined assembly method to encapsulate Coenzyme Q10(Co-Q10),a promising hydrophobic antioxidant which targets mitochondria ROS,into the lecithin micelles,which renders the insoluble Co-Q10 dispersible in water as stable colloids.These micelles are injectable,which displayed efficient ability to facilitate Co-Q10 to get into BMSCs in vitro,and exhibited prolonged release of Co-Q10 in intervertebral disc tissue of animal models.Compared to mere use of Co-Q10,the Co-Q10 loaded micelle possessed better bioactivities,which elevated the viability,restored mitochondrial structure as well as function,and enhanced production of ECM components in rat BMSCs.Moreover,it is demonstrated that the injection of this micelle with BMSCs retained disc height and alleviated IVDD in a rat needle puncture model.Therefore,these Co-Q10 loaded micelles play a protective role in cell survival and differentiation through antagonizing mitochondrial ROS,and might be a potential therapeutic agent for IVDD.

关键词： Intervertebral disc degeneration Coenzyme Q10 Mesenchymal stem cell Reactive oxygen species micelle

Highly stable hybrid single-micelle:A universal nanocarrier for hydrophobic bioimaging agents

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Nano Research 2022年第5期15卷 4582-4589页

作者： Qiaoyu Zhou Tiancong Zhao Mengli Liu Dongrui Yin Minchao Liu Ahmed AElzatahry Fan Zhang Dongyuan Zhao Xiaomin Li Department of Chemistry State Key Laboratory of Molecular Engineering of PolymersiChemShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200433China Materials Science and Technology Program College of Arts and SciencesQatar UniversityPO Box 2713DohaQatar

As the first-line technology,micelles play a pivotal role in in vivo delivery of theranostic agents because of their high biocompatibility and universality.However,in complex physiological environments(extreme dilution,pH,and oxidation or reduction,etc.),they generally suffer from structural instability and insufficient protection for encapsulated cargos.It is urgent to reinforce the structural stability of the micelles at the single-micelle level.By using the FDA-approved Pluronic F127 surfactants and indocyanine green(ICG)bioimaging agents as model,herein,we propose the silane-crosslinking assisted strategy to reinforce the structural stability of the single-micelle.Different from the traditional silane hydrolysis under the harsh experimental conditions(acidic,alkaline,and high temperature hydrothermal,etc.),the ICG loaded F127@SiO_(2) hybrid single-micelles(ICG@H-micelles)with controllable sizes(15-35 nm)are synthesized at neutral pH and room temperature,which is crucial for the maintenance of the physicochemical properties of the encapsulated cargos.With the ultra-thin SiO_(2)(micelle,the structural and fluorescence stability of ICG@H-micelles are much higher than the conventional micelle(ICG@micelles)in the simulated physiological environments of dilution,oxidation or reduction,and low pH.Because of the high structural and fluorescence stability,the ICG@H-micelles also exhibit longer duration time in the tumor and gastrointestinal tract bioimaging.

关键词： micelle SiO_(2) inorganic-organic hybrid mesoporous material bioimaging

Corrigendum to“Delivery of coenzyme Q10 loaded micelle targets mitochondrial ROS and enhances efficiency of mesenchymal stem cell therapy in intervertebral disc degeneration”[Bioact.Mater.23(2023)247-260]

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Bioactive Materials 2023年第6期24卷 171-173页

This corrects the article“Delivery of coenzyme Q10 loaded micelle targets mitochondrial ROS and enhances efficiency of mesenchymal stem cell therapy in intervertebral disc degeneration”in volume 23 on page 247.The authors regret that the printed version of the above article contains some errors which are not identified during the proofing stage.

关键词： loaded micelle coenzyme

A BRD4 PROTAC nanodrug for glioma therapy via the intervention of tumor cells proliferation,apoptosis and M2 macrophages polarization

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Acta Pharmaceutica Sinica B 2022年第6期12卷 2658-2671页

作者： Tingting Yang Yuzhu Hu Junming Miao Jing Chen Jiagang Liu Yongzhong Cheng Xiang Gao Department of Neurosurgery and Institute of Neurosurgery State Key Laboratory of Biotherapy and Cancer CenterWest China HospitalWest China Medical SchoolSichuan University and Collaborative Innovation Center for BiotherapyChengdu 610041China Department of Medical Oncology State Key Laboratory of Biotherapy and Cancer CenterWest China HospitalWest China Medical SchoolSichuan University and Collaborative Innovation Center for BiotherapyChengdu 610041China

Glioma is a primary aggressive brain tumor with high recurrence rate.The poor efficiency of chemotherapeutic drugs crossing the blood-brain barrier(BBB) is well-known as one of the main challenges for anti-glioma therapy.Moreover,massive infiltrated tumor-associated macrophages(TAMs) in glioma further thwart the drug efficacy.Herein,a therapeutic nanosystem(SPP-ARV-825) is constructed by incorporating the BRD4-degrading proteolytic targeting chimera(PROTAC) ARV-825 into the complex micelle(SPP) composed of substance P(SP) peptide-modified poly(ethylene glycol)-poly(D,L-lactic acid)(SP-PEG-PDLL A) and methoxy poly(ethylene glycol)-poly(D,L-lac tic acid)(mPEG-PDLL A,PP),which could penetrate BBB and target brain tumor.Subsequently,released drug engenders antitumor effect via attenuating cells proliferation,inducing cells apoptosis and suppressing M2 macrophages polarization through the inhibition of IRF4 promoter transcription and phosphorylation of STAT6,STAT3 and AKT.Taken together,our work demonstrates the versatile role and therapeutic efficacy of SPP-ARV-825 micelle against glioma,which may provide a novel strategy for glioma therapy in future.

关键词： Glioma BRD4 ARV-825 micelle M2 macrophage

Homopolypeptide Vesicles Triggered by Side-Chain Hydration

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Chinese Journal of Polymer Science 2022年第12期40卷 1631-1639,I0009页

作者： Xin-Jie Shi Zhen Liu Yang-Chun Xie Min Xu Xiao-Hua He School of Chemistry and Molecular Engineering East China Normal UniversityShanghai 200241China School of Physics and Electronic Science Shanghai Key Laboratory of Magnetic ResonanceEast China Normal UniversityShanghai 200241China

The formation of homopolypeptide vesicles and the identification of their self-assembly mechanism have been challenging issues in the field of polymer self-assembly. Using complementary circular dichroism(CD), Fourier transform infrared(FTIR) and low-field nuclear magnetic resonance(LF-NMR) spectroscopies, in this study we show that the higher hydrophilic ability of side-chains is a key factor for the formation of homopolypeptide vesicles from homo poly(Nε-carbobenzoxy-L-lysine)(PZlys), in which the vesicular structures are confirmed by scanning electron microscopy(SEM), transmission electron microscopy(TEM) and atomic force microscopy(AFM) measurements. Poly(γ-benzyl-Lglutamate-co-Nε-carbobenzoxy-L-lysine) [P(BLG-co-Zlys)] containing different molar ratios of BLG to Zlys units with the same peptide backbone as PZlys are used as the controls. The copolypeptides can only form micelles under the same conditions, due to the more hydrophobic nature of their side-chains. These results show that the specific side-chain structure of the polypeptides plays a fundamental role in the self-assembly of homopolypeptides. These findings can be useful to understand how the hydrophilicity of the side chains of amino acid residues on the surface of a protein affects its structures.

关键词： Polypeptide Vesicle Self-assembly Hydrophobic micelle

Strategies to improve micelle stability for drug delivery

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Nano Research 2018年第10期11卷 4985-4998页

作者： Yang Lu Ershuai Zhang Jianhai Yang Zhiqiang Cao Department of Chemical Engineering and Materials Science Wayne State University Detroit 48202 MI USA

micelles have been studied as drug delivery carriers for decades. Their use can potentially result in high drug accumulation at the target site through the enhanced permeability and retention effect. Nevertheless, the lack of stability of micelles in the physiological environment limits their efficacy as a drug carrier. In particular, micelles tend to disassociate and prematurely release the encapsulated drugs, lowering delivery efficacy and creating toxicity concerns. Many efforts to enhance the stability of micelles have focused mainly on decreasing the critical micelle forming concentration and improving blood circulation. Herein, we review different strategies including crosslinking and non-crosslinking approaches designed to stabilize micelles and offer perspectives on future research directions.

关键词： micelle stability crosslinking critical micelle concentration （CMC） drug delivery

Tumor microenvironment-responsive docetaxel-loaded micelle combats metastatic breast cancer

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Science Bulletin 2019年第2期64卷 91-100页

作者： Tianqun Lang Xinyue Dong Zhong Zheng Yiran Liu Guanru Wang Qi Yin Yaping Li State Key Laboratory of Drug Research & Center of Pharmaceutics Shanghai Institute of Materia Medica Chinese Academy of Sciences School of Pharmacy University of Chinese Academy of Sciences Nano Science and Technology Institute University of Science and Technology of China College of Life Sciences Jilin University School of Pharmacy Yantai University

Efficient tumor-targeting drug delivery systems are urgently needed for treating metastatic breast cancer.In this work, a docetaxel(DTX)-loaded micelle(pDM) as the tumor-microenvironment-responsive delivery platform is developed. The micelle is composed of a pH-sensitive amphiphilic copolymer,poly((1,4-butanediol)-diacrylate-b-N,N-diisopropylethylenediamine)-polyethyleneimine(BD-PEI), and a matrix metalloproteinase(MMP)-responsive polymer, poly((1,4-butanediol)-diacrylate-b-N,N-diisopropy lethylenediamine)-peptide-polyethylene glycol(PEG)(BD-peptide-PEG). The PEG block of BD-peptidePEG will be split by MMPs at the tumor microenvironment, which leads to the change of the surface charge and particle size of the micelle to more positive and smaller one. Owing to this transformation and enhanced permeability and retention(EPR) effect, pDM delivers more DTX into tumor tissues and is internalized more efficiently by tumor cells than the non-MMP-sensitive micelles in the 4 T1 tumorbearing mice model. In addition, DTX is released in acidic endo/lysosomes due to the dissociation of the micelle, triggered by the protonation of the hydrophobic block of BD-PEI. As a result, the DTX-loaded micelle inhibits primary tumor growth and pulmonary metastasis effectively. Thus, this pH/MMP-dual-sensitive drug delivery system, which simultaneously attains three keypoints: prolonged circulation time, directional and efficient uptake into tumor cells, and speedy intracellular drug release, is a promising strategy for metastatic breast cancer therapy.

关键词： Breast cancer Dual-sensitive micelle Metastasis Tumor-targeting