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Development of exosome membrane materialsfused microbubbles for enhanced stability and efficient Drug delivery of ultrasound contrast agent

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Acta Pharmaceutica Sinica B 2023年第12期13卷 4983-4998页

作者： Yongho Jang Jeehun Park Pilsu Kim Eun-Joo Park Hyungjin Sun Yujin Baek Jaehun Jung Tai-kyong Song Junsang Doh Hyuncheol Kim Department of Chemical and Biomolecular Engineering Sogang UniversitySeoul 04107Republic of Korea Research Institute of Advanced Materials(RIAM) Institute of Engineering ResearchSeoul National UniversitySeoul 08826Republic of Korea Department of Electronic Engineering Sogang UniversitySeoul 04107Republic of Korea Biomedical Research Institute&Department of Radiology Seoul National University HospitalSeoul 03080Republic of Korea Interdisciplinary Program in Bioengineering Seoul National UniversitySeoul 08826Republic of Korea Department of Materials Science and Engineering Seoul National UniversitySeoul 08826Republic of Korea Institute of Engineering Research Bio-MAX InstituteSeoul National UniversitySeoul 08826Republic of Korea Department of Biomedical Engineering Sogang UniversitySeoul 04107Republic of Korea

Lipid-coated microbubbles are widely used as an ultrasound contrast agent,as well as Drug delivery carriers.However,the two main limitations in ultrasound diagnosis and Drug delivery using microbubbles are the short half-life in the blood system,and the difficulty of surface modification of microbubbles for active targeting.The exosome,a type of extracellular vesicle,has a preferentially targeting ability for its original cell.In this study,exosome-fused microbubbles(Exo-MBs)were developed by embedding the exosome membrane proteins into microbubbles.As a result,the stability of Exo-MBs is improved over the conventional microbubbles.On the same principle that under the exposure of ultrasound,microbubbles are cavitated and self-assembled into nano-sized particles,and Exo-MBs are self-assembled into exosome membrane proteins-embedded nanoparticles(Exo-NPs).The Exo-NPs showed favorable targeting properties to their original cells.A photosensitizer,chlorin e6,was loaded into Exo-MBs to evaluate therapeutic efficacy as a drug carrier.Much higher therapeutic efficacy of photodynamic therapy was confirmed,followed by cancer immunotherapy from immunogenic cell death.We have therefore developed a novel ultrasound image-guided Drug delivery platform that overcomes the shortcomings of the conventional ultrasound contrast agent and is capable of simultaneous photodynamic therapy and cancer immunotherapy.

关键词： Exosomes Microbubbles Photodynamic therapy Ultrasound Sonoporation Cancer immunotherapy Drug delivery

Bioinspired drug-delivery system emulating the natural bone healing cascade for diabetic periodontal bone regeneration

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Bioactive Materials 2023年第3期21卷 324-339页

作者： He Wang Xiaowei Chang Qian Ma Boyang Sun Han Li Jinmin Zhou Yiyao Hu Xiaoyu Yang Jie Li Xin Chen Jinlin Song Chongqing Key Laboratory of Oral Diseases and Biomedical Sciences Chongqing Municipal Key Laboratory of Oral Biomedical Engineering of Higher EducationCollege of Stomatology of Chongqing Medical UniversityChongqing401147China Department of Chemical Engineering Shaanxi Key Laboratory of Energy Chemical Process IntensificationInstitute of Polymer Science in Chemical EngineeringSchool of Chemical Engineering and TechnologyXi′an Jiaotong UniversityXi′an710049China

Diabetes mellitus(DM)aggravates periodontitis,resulting in accelerated periodontal bone resorption.Disordered glucose metabolism in DM causes reactive oxygen species(ROS)overproduction resulting in compromised bone healing,which makes diabetic periodontal bone regeneration a major challenge.Inspired by the natural bone healing cascade,a mesoporous silica nanoparticle(MSN)-incorporated PDLLA(poly(DL-lactide))-PEG-PDLLA(PPP)thermosensitive hydrogel with stepwise cargo release is designed to emulate the mesenchymal stem cell“recruitment-osteogenesis”cascade for diabetic periodontal bone regeneration.During therapy,SDF-1 quickly escapes from the hydrogel due to diffusion for early rat bone marrow stem cell(rBMSC)recruitment.Simulta-neously,slow degradation of the hydrogel starts to gradually expose the MSNs for sustained release of metformin,which can scavenge the overproduced ROS under high glucose conditions to reverse the inhibited osteogenesis of rBMSCs by reactivating the AMPK/β-catenin pathway,resulting in regulation of the diabetic microenvironment and facilitation of osteogenesis.In vitro experiments indicate that the hydrogel markedly restores the inhibited migration and osteogenic capacities of rBMSCs under high glucose conditions.In vivo results suggest that it can effectively recruit rBMSCs to the periodontal defect and significantly promote periodontal bone regeneration under type 2 DM.In conclusion,our work provides a novel therapeutic strategy of a bioinspired drug-delivery system emulating the natural bone healing cascade for diabetic periodontal bone regeneration.

关键词： Periodontal bone regeneration Diabetes mellitus Bioinspired Hydrogel Drug delivery

Wearable patches for transdermal Drug delivery

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药学学报:英文版 2023年第6期13卷 2298-2309页

作者： Jiahui He Yuyue Zhang Xinge Yu Chenjie Xu Department of Biomedical Engineering City University of Hong KongHong Kong 999077China Hong Kong Centre for Cerebro-Cardiovascular Health Engineering Hong Kong 999077China

Transdermal Drug delivery systems(TDDs) avoid gastrointestinal degradation and hepatic first-pass metabolism, providing good drug bioavailability and patient compliance. One emerging type of TDDs is the wearable patch worn on the skin surface to deliver medication through the skin. They can generally be grouped into passive and active types, depending on the properties of materials,design principles and integrated devices. This review describes the latest advancement in the development of wearable patches, focusing on the integration of stimulus-responsive materials and electronics.This development is deemed to provide a dosage, temporal, and spatial control of therapeutics delivery.

关键词： Wearable patch Transdermal delivery Microneedles Drug delivery Biomaterials

Microneedle patch loaded with ferritin-nanocaged doxorubicin for locally targeted Drug delivery and efficient skin cancer treatment

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Particuology 2024年第5期88卷 282-289页

作者： Feng Li Yuan Yang Hua Yue Shuang Wang Xiao Zhang Wei Wei State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China Key Laboratory of Biopharmaceutical Preparation and delivery Chinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Ferritin has emerged as a promising nanocarrier for delivering therapeutic agents to tumours.However,the limited drug loading and the off-target impacts after systemic administration remain challenges for cancer treatment with ferritin-based agents.Herein,we develop a microneedle patch loaded with ferritin-nanocaged doxorubicin(DoxFe@Fn/MN)for skin cancer treatment.Briefly,doxorubicin(Dox)is encapsulated in ferritin(Fn)using an iron core-assisted strategy,which results in a 3.4-fold increase in Dox loading compared to the direct loading method.Then,a polyvinyl alcohol-based microneedle(MN)patch is used for the transdermal delivery of DoxFe@Fn,enabling targeted tumour accumulation of DoxFe@Fn and preventing off-target impacts.The released DoxFe@Fn can bind to CD71 highly expressed on skin cancer cells,facilitating its uptake.As a result,the DoxFe@Fn/MN therapy presents a robust antitumour effect in a melanoma tumour model,showing its potential as a promising therapeutic modality for skin cancer treatment.

关键词： Ferritin Microneedle Skin cancer Drug delivery

Cyclic arginine-glycine-aspartic acid-modified red blood cells for Drug delivery:Synthesis and in vitro evaluation

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Journal of Pharmaceutical Analysis 2022年第2期12卷 324-331页

作者： Chen Wang Min Wang Yan Zhang Hongxin Jia Binbin Chen Department of Pharmaceutics School of PharmacyXiamen Medical CollegeXiamenFujian361023China Institute of Respiratory Diseases Xiamen Medical CollegeXiamenFujian361023China Department of Pharmaceutics School of PharmacyHarbin University of CommerceHarbin150076China Department of Pharmacy Xiamen Xianyue HospitalXiamenFujian361012China

Red blood cells(RBCs)are an excellent choice for cell preparation research because of their biocompatibility,high drug loading,and long half-life.In this study,doxorubicin(DOX)was encapsulated with RBCs as the carrier.The biotin-avidin system binding principle was used to modify biotinylated cyclic arginine-glycine-aspartic acid(cRGD)onto RBC surfaces for accurate targeting,high drug loading,and sustained drug release.The RBC Drug delivery system(DDS)was characterized,and the concentration of surface sulfur in the energy spectrum was 6.330%.The physical and chemical properties of RBC DDS were as follows:drug content,0.857 mg/mL;particle size,3339 nm;potential value,12.5 mV;and cumulative release rate,81.35%.There was no significant change in RBC morphology for up to seven days.The results of the targeting and cytotoxicity studies of RBC DDS showed that many RBCs covered the surfaces of U251 cells,and the fluorescence intensity was higher than that of MCF-7 cells.The IC50 value of unmodified drug-loaded RBCs was 2.5 times higher than that of targeted modified drug-loaded RBCs,indicating that the targeting of cancer cells produced satisfactory inhibition.This study confirms that the RBC DDS has the characteristics of accurate targeting,high drug loading,and slow drug release,which increases its likelihood of becoming a clinical cancer treatment in the future.

关键词： Cytotoxicity Red blood cells Drug delivery Targeting

Carvacrol combined with NIR light-responsive nano-Drug delivery system with specific anti-bacteria,anti-inflammation,and immunomodulation for periodontitis

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Nano Research 2023年第5期16卷 7199-7215页

作者： Daorun Hu Congkai Zhang Chao Sun Haijing Bai Jialiang Xie Yawen Gu Mengyuan Li Junkai Jiang Aiping Le Jiaxuan Qiu Xiaolei Wang Department of Oral and Maxillofacial Surgery The First Affiliated Hospital of Nanchang UniversityNanchang 330006China The National Engineering Research Center for Bioengineering drugs and the Technologies Institute of Translational MedicineNanchang UniversityNanchang 330088China Department of Transfusion Medicine The First Affiliated Hospital of Nanchang UniversityKey Laboratory of Jiangxi Province for Transfusion MedicineThe First Affiliated Hospital of Nanchang UniversityNanchang 330006China College of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330088China

Bacterial infection,biofilm formation,immune dysfunction are common triggers and aggravators in periodontitis,which render periodontal restoration challenging.Thus,a strategy with antibacterial,anti-inflammatory,immunoregulatory capacities has great promise in the clinical practice of periodontitis.Herein,carvacrol(CA)-based near-infrared(NIR)lightresponsive nano-Drug delivery system is developed for the first time.The system consists of upconversion nanoparticles(UCNPs,which upconvert 808 nm NIR to blue light),mesoporous silica(mSiO_(2),the carrier channel),hydrophobic CA(blue light response properties).Under the irradiation of 808 nm NIR,owing to the synergy of CA and upconverted blue light,the UCNPs@mSiO_(2)-CA(UCMCs)exhibit the properties of specific anti-bacteria(including anaerobic bacteria),anti-inflammation,and immunomodulation.Notably,high-throughput sequencing results exhibit that many classic inflammatory immune-related signaling pathways,including the MAPK signaling pathway,tumor necrosis factor(TNF)signaling pathway,IL-17 signaling pathway,are enriched to remodel the immune microenvironment.Additionally,UCMCs with NIR irradiation accelerate periodontal restoration and serve as promising non-invasive management of periodontitis.Altogether,this study verifies the feasibility of herbal monomer combined with light-responsive in situ nano-Drug delivery system and provides a more effective and reliable strategy for various potential applications of deep tissue diseases.

关键词： anti-bacteria near-infrared light upconversion nanoparticle periodontitis Drug delivery

Engineered self-healing single-cavity microcapsules for pulsatile release of Drug delivery

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Particuology 2023年第9期80卷 53-60页

作者： Tong Ye Lingjiao Zou Yishu Wang Guanghui Ma State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Division of Molecular Science Graduate School of Science and TechnologyGunma University1-5-1Tenjin-choKiryu376-8515Japan Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing100190China

A wide range of polymer-based Drug delivery systems have been reported for the treatment of variousdiseases.However,the dosing regimen of many drugs,such as stimulator of interferon genes agonists,programmed cell death protein-1 antibodies,and coronavirus disease 2019 vaccines,consists of repeatedintratumoral or intramuscular injections.These repeated administrations may lead to poor adherence,thus resulting in compromised therapeutic outcomes and increased financial burden.Here,we developed a multidose Drug delivery platform by engineering polylactic-co-glycolic acid(PLGA)with differentmolecular weights into self-healing single-cavity microcapsules(SSM).This approach showed a flexiblecollocation strategy to achieve customized pulsatile drug release and was fully degradable with goodsafety.Notably,this single-injection delivery system contains only PLGA,holding great promise forclinical translation.

关键词： Drug delivery Single-cavity microcapsule Pulsatile release Self-healing microparticle

Magnetically responsive nanofibrous ceramic scaffolds for on-demand motion and Drug delivery

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Bioactive Materials 2022年第9期7卷 372-381页

作者： Yonggang Zhang Jiaping Li Pamela Habibovic Department of Instructive Biomaterials Engineering Maastricht UniversityMERLN Institute for Technology-Inspired Regenerative MedicineUniversiteitssingel 406229 ERMaastrichtthe Netherlands Department of Complex Tissue Regeneration Maastricht UniversityMERLN Institute for Technology-Inspired Regenerative MedicineUniversiteitssingel 406229 ERMaastrichtthe Netherlands

Smart biomaterials,featuring not only bioactivity,but also dynamic responsiveness to external stimuli,are desired for biomedical applications,such as regenerative medicine,and hold great potential to expand the boundaries of the modern clinical practice.Herein,a magnetically responsive three-dimensional scaffold with sandwich structure is developed by using hydroxyapatite(HA)nanowires and ferrosoferric oxide(Fe_(3)O_(4))nanoparticles as building blocks.The magnetic HA/Fe_(3)O_(4) scaffold is fully inorganic in nature,but shows polymeric hydrogel-like characteristics including a 3D fibrous network that is highly porous(>99.7%free volume),deformable(50%deformation)and elastic,and tunable stiffness.The magnetic HA/Fe3O4 scaffold has been shown to execute multimodal motion upon exposure to an external magnetic field including shape transformation,rolling and somersault.In addition,we have demonstrated that the magnetic scaffold can serve as a smart carrier for remotely controlled,on-demand delivery of compounds including an organic dye and a protein.Finally,the magnetic scaffold has exhibited good biocompatibility,supporting the attachment and proliferation of human mesenchymal stromal cells,thereby showing great potential as smart biomaterials for a variety of biomedical applications.

关键词： Hydroxyapatite Magnetic Responsive Drug delivery Cell culture

MMP-2 and upconverted UV dual-mediated drug sequential delivery and on-site immobilization for enhanced multidrugresistant cancer therapy

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Science China Chemistry 2023年第8期66卷 2317-2328页

作者： Anna Wang Jing Fang Yali Feng Yuqi Zhang Yan Zhao Jiachen Li Chaoxiang Cui Yi Hou Haibin Shi Mingyuan Gao State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Centre of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou215123China Institute of Chemistry Chinese Academy of Sciences Beijing100190China

Controlled Drug delivery holds great potential for effective tumor treatment owing to the merits of overcoming drug resistance and improving therapeutic efficacy while minimizing systemic toxicity.However,accurate and controllable delivery of chemotherapeutics into tumor tissue with high efficiency remains a huge challenge.Taking advantage of the UV-emitting characteristics of upconversion nanoparticles(UCNPs),herein we for the first time report an MMP-2 enzyme and near infrared(NIR)dual-mediated sequential Drug delivery and in-situ immobilization(ENDDI)system that is fabricated by decorating UCNPs with MMP-2 responsive and photocrosslinkable peptide bearing anticancer drug doxorubicin(DOX)for overcoming multidrug resistance.Upon cleavage with tumor-specific MMP-2,the peptide fragment containing a photolabile benzophenone(BP)and DOX could be released and in-situ immobilized within the tumor through the covalent crosslinking reaction between BP and neighboring biomolecules under the excitation of converted UVemission from UCNPs,which remarkably blocks the exocytosis of DOX leading to prolonged drug retention,achieving significant suppression of DOX-resistant breast tumors.Our current dual stimuli-mediated sequential Drug delivery and in-situ immobilization represent a generalizable strategy for the effective treatment of multidrug resistant tumors.

关键词： upconversion nanoparticles photocrosslinking Drug delivery in situ immobilization multidrug resistance