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Rod-shape inorganic biomimetic mutual-reinforcing MnO2-Au nanozymes for catalysis-enhanced hypoxic tumor therapy

Nano Research 2020年第8期13卷 2246-2258页

作者： Lifang Yang Chuchu Ren Min Xu Yilin Song Qianglan Lu Yule Wang Yan Zhu Xinxing Wang Nan Li Tianjin Key Laboratory of Drug Delivery&High-Efficiency School of Pharmaceutical Science and TechnologyTianjin UniversityTianjin300072China Tianjin State Key Laboratory of Modern Chinese Medicine Tianjin University of Traditional Chinese MedicineBeihua South RoadJingHai DistrictTianjin301617China Research and Development Center of TCM Tianjin International Joint Academy of Biotechnology and Medicine220 Dongting RoadTEDATianjin300457China Tianjin Institute of Environmental and Operational Medicine 1 Dali RoadHeping DistrictTianjin300050China

Biomimetic nanozymes possessing natural enzyme-mimetic activities have been extensively applied in nanocatalytic tumor ***,engineering hybrid biomimetic nanozymes to achieve superior nanozyme activity remained to be an intractable challenge in hypoxic ***,a rod-like biomimetic hybrid inorganic MnO2-Au nanozymes are developed,where MnO2 and ultrasmall Au nanoparticles(NPs)are successively deposited on the mesoporous silica nanorod to cooperatively improve the O2 content and thermal sensitivity of hypoxic solid tumors guided by multi-modal *** the catalyzing of MnO2,the intratumoral H2O2 is decomposed to greatly accelerate O2 generation,which could boost the curative effect of radiation therapy(RT)and further enhance the Au-catalyzed glucose ***,the Au NPs can steadily and efficiently catalyze the oxidation of glucose in harsh tumor microenvironment,thus sensitizing tumor cells to thermal ablation for mild photothermal therapy and further promoting the catalytic efficiency of MnO2 with the self-supplied H2O2/H+.As a result,this mutual-reinforcing cycle can endow the nanoplatform with accelerated O2 generation,thus alleviating hypoxic environment and further boosting RT ***,acute glucose consuming can induce downregulation expression of heat shock protein(HSP),achieving starvation-promoted mild photothermal *** synthesized hybrid nanozymes proves to be a versatile theranostic agent for nanocatalytic cancer therapy.

关键词： nanozyme self-supplied mutual-reinforcing hypoxia catalysis-enhanced therapy

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Silk-based hydrogel incorporated with metal-organic framework nanozymes for enhanced osteochondral regeneration

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Bioactive Materials 2023年第2期20卷 221-242页

作者： Zhicheng Cao Hongmei Wang Jialin Chen Yanan Zhang Qingyun Mo Po Zhang Mingyue Wang Haoyang Liu Xueyang Bao Yuzhi Sun Wei Zhang Qingqiang Yao Department of Orthopaedic Surgery Institute of Digital MedicineNanjing First HospitalNanjing Medical University210006NanjingChina School of Medicine Southeast University210009NanjingChina Department of Pharmaceutical Sciences Binzhou Medical University264003YantaiShandongChina Jiangsu Key Laboratory for Biomaterials and Devices Southeast University210096NanjingChina China Orthopedic Regenerative Medicine Group(CORMed) China

Osteochondral defects(OCD)cannot be efficiently repaired due to the unique physical architecture and the pathological microenvironment including enhanced oxidative stress and *** strategies,such as the control of implant microstructure or the introduction of growth factors,have limited functions failing to manage these complex *** we developed a multifunctional silk-based hydrogel incorporated with metal-organic framework nanozymes(CuTA@SF)to provide a suitable microenvironment for enhanced OCD *** incorporation of CuTA nanozymes endowed the SF hydrogel with a uniform microstructure and elevated *** vitro cultivation of mesenchymal stem cells(MSCs)and chondrocytes showed that CuTA@SF hydrogel accelerated cell proliferation and enhanced cell viability,as well as had antioxidant and antibacterial *** the inflammatory environment with the stimulation of IL-1β,CuTA@SF hydrogel still possessed the potential to promote MSC osteogenesis and deposition of cartilage-specific extracellular matrix(ECM).The proteomics analysis further confirmed that CuTA@SF hydrogel promoted cell proliferation and ECM *** the full-thickness OCD model of rabbit,CuTA@SF hydrogel displayed successfully in situ OCD regeneration,as evidenced by micro-CT,histology(HE,S/O,and toluidine blue staining)and immunohistochemistry(Col I and aggrecan immunostaining).Therefore,CuTA@SF hydrogel is a promising biomaterial targeted at the regeneration of OCD.

关键词： Osteochondral regeneration Metal-organic framework nanozyme Inflammation ROS Silk

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Remodeling of the liver fibrosis microenvironment based on nilotinib-loaded multicatalytic nanozymes with boosted antifibrogenic activity

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Acta Pharmaceutica Sinica B 2023年第12期13卷 5030-5047页

作者： Huaqing Jing Yingzi Ren Yue Zhou Min Xu Sona Krizkova Zbynek Heger Qiang Lu Siyu Wang Xiaoyang Liang Vojtech Adam Nan Li Tianjin Key Laboratory of Drug Delivery&High-Eficiency School of Pharmaceutical Science and TechnologyTianjin UniversityTianjin 300072China Department of Chemistry and Biochemistry Mendel University in BrnoBrno 61300Czech Republic

Liver fibrosis is a reversible pathological process caused by chronic liver damage and a major risk factor for hepatocellular carcinoma(HCC).Hepatic stellate cell(HSC)activation is considered the main target for liver fibrosis ***,the efficiency of this strategy is limited due to the complex microenvironment of liver fibrosis,including excessive extracellular matrix(ECM)deposition and hypoxia-induced imbalanced ECM ***,nilotinib(NIL)-loaded hyaluronic acid(HA)-coated Ag@Pt nanotriangular nanozymes(APNH NTs)were developed to inhibit HSCs activation and remodel the microenvironment of liver *** NTs efficiently eliminated intrahepatic reactive oxygen species(ROS)due to their inherent superoxide dismutase(SOD)and catalase(CAT)activities,thereby downregulating the expression of NADPH oxidase-4(NOX-4)and inhibiting HSCs ***,the oxygen produced by the APNH NTs further alleviated the hypoxic ***,the released NIL promoted collagen depletion by suppressing the expression of tissue inhibitor of metalloproteinase-1(TIMP-1),thus synergistically remodeling the microenvironment of liver ***,an in vivo study in CCl_(4)-induced mice revealed that APNH NTs exhibited significant antifibrogenic effects without obvious long-term *** together,the data from this work suggest that treatment with the synthesized APNH NTs provides an enlightening strategy for remodeling the microenvironment of liver fibrosis with boosted antifibrogenic activity.

关键词： Liver fibrosis Microenvironment remodeling HSCs ECM Collagen Hypoxia Nilotinib nanozyme

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Molecular insights of nanozymes from design to catalytic mechanism

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Science China Chemistry 2023年第5期66卷 1318-1335页

作者： Yuan Xu Zhixin Zhou Nankai Deng Kangchun Fu Caixia Zhu Qing Hong Yanfei Shen Songqin Liu Yuanjian Zhang Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical ResearchSchool of Chemistry and Chemical EngineeringMedical SchoolSoutheast UniversityNanjing 21l189China

Emerging as cost-effective potential alternatives to natural enzymes,nanozymes have attracted increasing interest in broad *** exploit the in-depth potential of nanozymes,rational structural engineering and explicit catalytic mechanisms at the molecular scale are ***,impressive progress has been made in mimicking the characteristics of natural enzymes by constructing metal active sites,binding pockets,scaffolds,and delicate allosteric *** in-depth studies have been conducted with advances in structural characterization and theoretical calculations,unveiling the“black box”of nanozymecatalytic *** review introduces the state-of-art synthesis strategies by learning from the natural enzyme counterparts and summarizes the general overview of the nanozyme mechanism with a particular emphasis on the adsorbed intermediates and descriptors that predict the nanozyme *** emerging activity assessment methodology that illustrates the relationship between electrochemical oxygen reduction and enzymatic oxygen reduction is discussed with up-to-date *** opportunities and challenges are presented in the end to spark more profound work and attract more researchers from various backgrounds to the flourishing field of nanozymes.

关键词： nanozyme mechanism descriptor free-ROS bound-ROS

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Advances in Single-Atom nanozymes Research

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Chinese Journal of Chemistry 2021年第1期39卷 174-180页

作者： Bing Jiang Minmin Liang Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

nanozymes with intrinsic enzyme-like properties have attracted significant interest owing to their capability to address the limitations of traditional enzymes such as fragility,high cost and dificult mass ***,the currently reported nanozymes are generally less active than natural *** recent years,with the rapid development of nanoscience and nanotechnology,single-atom nanozymes(SAzymes)with well-defined electronic and geometric structures have shown a promise to serve as direct surrogates of traditional enzymes by mimicking the highly evolved catalytic center of natural *** this review,we will introduce the enzymatic characteristics and recent advances of SAzymes,and summarize their significant applications from in vitro detection to in vivo monitoring and therapy.

关键词： nanozyme Single-atom nanozyme Biomedical application

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Recent progress in carbon-dots-based nanozymes for chemosensing and biomedical applications

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Chinese Chemical Letters 2021年第10期32卷 2994-3006页

作者： Deming He Minmin Yan Pengjuan Sun Yuanqiang Sun Lingbo Qu Zhaohui Li College of Chemistry Green Catalysis CenterHenan Joint International Research Laboratory of Green Construction of Functional Molecules and Their Bioanalytical ApplicationsZhengzhou Key Laboratory of Functional Nanomaterial and Medical TheranosticZhengzhou UniversityZhengzhou 450001China

nanozymes are nanomaterials with enzyme-like activities that efficiently overcome the drawbacks of natural enzymes in biosensing,detection,and biomedical fields,and they are the most widely used artificial *** to their excellent catalytic characteristics,biocompatibility,and environmental favorability,carbondots-based(CDs) nanozymes have inspired a research ***,no review focusing on CDs nanozymes has been published,even though substantial advances have been ***,the advances,catalytic activities,and applications of CDs nanozymes are highlighted and *** addition,the critical issues and challenges of researching nanozymes are *** hope that this review will broaden the horizons of nanozymes and CDs nanozymes,as well as promote their development.

关键词： Carbon dots nanozyme Chemosensing Catalytic activity Bioimaging

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Emerging nanozymes for potentiating radiotherapy and radiation protection

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Chinese Chemical Letters 2022年第7期33卷 3315-3324页

作者： Yu Chong Jiayu Ning Shengyi Min Jiaquan Ye Cuicui Ge State Key Laboratory of Radiation Medicine and Protection School of Radiation Medicine and ProtectionSchool for Radiological and Interdisciplinary Sciences(RAD-X)Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China

While radiotherapy is a mainstay therapeutic modality for malignant tumor,the intrinsic tumor resistance to radiotherapy,as well as the concomitant radiation injury to adjacent healthy tissues,greatly limits the efficacy of cancer *** a result,the development of novel radioenhancers and radioprotectants is highly desired for clinical *** recent years,nanozymes have inspired ever-growing research interest because of their multi-enzyme activities and microenvironment-responsive *** view of the significant progress of nanozymes in radiation medicine,we,in this review,systematically illustrate the impressive progress of nanozymes for potentiating radiotherapy and radiation ***,the types of nanozymes used in tumor radiotherapy are briefly ***,the main strategies of nanozymes to enhance the radiotherapy efficiency,including promoting the generation of reactive oxygen species(ROS),relieving hypoxia in tumor microenvironment and combining with other cancer therapeutic regimens,are ***,the advances of typical nanozymes for preventing radiation-induced hematopoietic damage and gastrointestinal damage are highlighted.

关键词： nanozyme Radiation therapy Radiosensitization ROS Hypoxia

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Fluorescent MOF-based nanozymes for discrimination of phenylenediamine isomers and ratiometric sensing of o-phenylenediamine

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Chinese Chemical Letters 2022年第4期33卷 2081-2085页

作者： Yinghui Xia Kunming Sun Ya-Nan Zuo Shuyun Zhu Xian-En Zhao School of Chemistry and Chemical Engineering Qufu Normal UniversityQufu 273165China

Although peroxidase-like nanozymes have made great progress in bioanalysis,few current nanozymebased biosensors are constructed for discriminating isomers of organic ***,fluorescent metal-organic framework(MOF)-based nanozyme is utilized for phenylenediamine isomers discrimination and ***_(2)-MIL-101(Fe),as a member of Fe-based MOFs,functions as not only fluorescent indicator but also peroxidase *** the presence of H_(2)O_(2),NH2-MIL-101(Fe) can catalyze the oxidation of o-phenylenediamine(OPD) and p-phenylenediamine(PPD) into their corresponding oxidation products(OPDox and PPDox),which in turn quench its intrinsic fluorescence at 445 nm via inner filter effect(IFE).Differently,a new fluorescence peak at 574 nm is observed for ***,a ratiometric fluorescence method for the detection of OPD can be designed with the fluorescence intensity ratio F_(574)/F_(445)as *** proposed strategy displays excellent discrimination ability for three phenylenediamines and may open new applications of MOFs in environmental science.

关键词： Bifunctional MOF nanozyme Photoluminescence Aromatic diamine isomers Ratiometric fluorescence

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Modification and application of Fe_(3)O_(4) nanozymes in analytical chemistry:A review

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Chinese Chemical Letters 2023年第5期34卷 46-56页

作者： Jiahe Ju Yitong Chen Zhiqiang Liu Cheng Huang Yaqi Li Dezhao Kong Wei Shen Sheng Tang School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Grain Science and Technology Jiangsu University of Science and TechnologyZhenjiang 212003China

In recent years,Fe_(3)O_(4)nanomaterials have received much attention in analytical chemistry due to their excellent magnetic and peroxidase-like *** the catalytic characteristics of Fe_(3)O_(4)nanomaterials is similar to those of horseradish peroxidase(HRP),Fe_(3)O_(4)nanomaterials are also used as peroxidase mimics and have achieved a certain development in many fields based on latest research *** improve the stability and catalytic ability of simple Fe_(3)O_(4)nanomaterials,various modification strategies of Fe_(3)O_(4)nanomaterials have been *** recent advances of these strategies have been presented and *** addition,this paper introduces the application of Fe_(3)O_(4)nanozymes in the detection of food and industrial pollutants,as well as in the field of biosafety.

关键词： Fe_(3)O_(4)nanomaterials nanozyme Peroxidase-like activity Modification Application

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Theranostic nanosystem mediating cascade catalytic reactions for effective immunotherapy of highly immunosuppressive and poorly penetrable pancreatic tumor

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Science China Chemistry 2022年第7期65卷 1383-1400页

作者： Gengjia Chen Yujun Cai Bo Li Minzhao Lin Xiaobin Wang Zhiyong Wang Xintao Shuai Key Laboratory for Polymeric Composite&Functional Materials of Ministry of Education School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275China Nanomedicine Research Center the Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhou 510630China Department of Minimally Invasive Interventional Radiology Laboratory of Interventional Radiologythe Second Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510275China

The dense desmoplastic stroma and immunosuppressive microenvironment of pancreatic cancer hinder the penetration of drugs and induce a considerable resistance to conventional chemoradiotherapy. Although nanomedicine has recently shown attractive potential in cancer immunotherapy, it remains a great challenge to achieve efficient drug delivery and potent immune ***, a stimuli-responsive nanosystem, comprising superparamagnetic iron oxide nanocrystals and nitric oxide(NO) donors,was developed for in-situ triggered catalytic cascade reaction to produce abundant free radicals and remodel the anti-tumor immunity. The nanosystem was activated in the tumor microenvironment to produce NO which dilated the tumor vasculature for efficient drug delivery, and the iron oxide nanocrystals catalyzed the reaction of NO to generate reactive oxygen-nitrogen species(RONS) with high cytotoxicity. Moreover, owing to the catalytic cascade reactions mediated by the nanosystem, the tumor associated macrophages(TAMs) were converted to a proinflammatory M1 phenotype and tumor infiltration of effector T cells was promoted to result in potent anti-tumor immunotherapy which could be readily monitored with magnetic resonance imaging(MRI).

关键词： nanozyme catalytic cascade reactions macrophages tumor microenvironment nitric oxide

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