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A Mn-porphyrinic metal–organic framework immobilizing glucose oxidase for combined photodynamic/chemodynamic/starvation therapy

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Tungsten 2025年第1期7卷 183-194页

作者： Xin-Ran Sun Hao-Ming Yuan Guo-Da Zhang Chao Wang Shu-Juan Sun Peng-Fei Shi Shandong Provincial Key Laboratory of Detection Technology for Tumor Markers School of Chemistry and Chemical Engineering Linyi University

The combination of photodynamic therapy（PDT） and chemodynamic therapy（CDT） in tumor treatment has attracted considerable ***,tumor hypoxia and glutathione（GSH） overproduction in the tumor tissue restricted the progress of their ***,a Mn-porphyrinic metal-organic framework（Mn-TCPP） was constructed by the one-pot method and further used for immobilizing glucose oxidase（GOx） to obtain GOx@*** would rapidly exhaust endogenous glucose into hydrogen peroxide（H2O2） and gluconic acid,thus shutting off the energy supply of tumor cells for starvation ***-TCPP catalyzed H2O2to produce oxygen,regulating the hypoxic tumor microenvironment and in turn improving1O2generation under laser ***,Mn-TCPP can reduce reactive oxygen species consumption owing to the redox reaction between Mn3+and GSH,thus greatly enhancing ***,benefiting from GOx-mediated starvation therapy,Mn2+produced by Mn3+reduction can react with sufficient intracellular H2O2to generate ·OH with high cytotoxicity through a Fenton-like *** treatment by GOx@Mn-TCPP under laser irradiation in vitro,the cell viability of 4T1 and A549 tumor cells reached to 20%,reflecting GOx@Mn-TCPP could give full play to the advantages of PDT/CDT/starvation *** results in vivo demonstrated that GOx@Mn-TCPP mediated synergistic cascade therapy could significantly inhibit tumor growth and improve the therapeutic effect.

关键词： chemodynamic therapy Immobilizing enzyme Metal–organic frameworks Photodynamic therapy Starvation therapy

Light/pH dual controlled drug release"nanocontainer"alleviates tumor hypoxia for synergistic enhanced chemotherapy,photodynamic therapy and chemodynamic therapy

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Bio-Design and Manufacturing 2024年第6期7卷 955-971页

作者： Shihe Liu Xin Zhang Zhimin Bai Yibo Yang Jia Zhang Kun Li Zhiwei Liu Ming Shi Lixin Dong Jidong Wang Jian Li Hebei Key Laboratory of Applied Chemistry Hebei Key Laboratory of NanobiotechnologyHebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource ReuseYanshan UniversityQinhuangdao 066004China Qinhuangdao Biopha Biotechnology Co. Ltd.Qinhuangdao 066000China The First Hospital of Qinhuangdao Qinhuangdao 066000China Department of Biological Engineering College of Environment and Chemical EngineeringYanshan UniversityQinhuangdao 066004China

Photodynamic therapy(PDT)has significant advantages in treating primary ***,the hypoxic tumor microenvironment hinders the generation of sufficient reactive oxygen species during PDT to effectively kill tumor cells,further greatly limiting the applications of PDT in cancer ***,we reported a temperature/pH dual controlled drug delivery system LPC@PCN@PDA/Fe^(3+)-AS1411 based on a porous coordination network(PCN(Mn))coated with polydopamine(PDA)and modified with an aptamer AS1411.β-lapachone(LPC)was loaded inside the PCN(Mn)framework,and Fe^(3+)was attached to the surface of the PDA *** nanoparticles(NPs)exhibited excellent multimodal cancer therapeutic effects and tumor targeting ability with their photo-and chemodynamic *** therapeutic effect can be enhanced by the production of sufficient oxygen by the internal hydrogen peroxide,which improves the photodynamic effect of the photosensitizer PCN(Mn)and the chemotherapy effect ofβ-***,the conversion of Fe^(2+)to Fe^(3+)in the tumor cells exerts the Fenton effect,which generates hydroxyl radicals that cause lipid peroxidation in tumor cells and induce apoptosis,thus enhancing the chemodynamic therapeutic *** vitro and in vivo experiments revealed that the NPs demonstrated specific tumor targeting,excellent inhibition effect on tumor growth,and ***,our findings can help develop an intelligent multifunctional therapeutic nanoplatform for cancer therapy.

关键词： Porous coordination network(Mn)framework Phototherapy Photodynamic therapy chemodynamic therapy Fenton effect

Spatially asymmetric cascade nanocatalysts for enhanced chemodynamic therapy

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Nano Research 2023年第7期16卷 9642-9650页

作者： Minchao Liu Hongyue Yu Liang Chen Tiancong Zhao Meng Fang Mengli Liu Qiaoyu Zhou Fatemah Farraj AlHarbi Ahmed Mohamed El-Toni 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 Department of Musculoskeletal Cancer Surgery Fudan University Shanghai Cancer CenterShanghai 200032China Department of Physics College of SciencePrincess Nourah bint Abdulrahman UniversityP.O.Box 84428Riyadh 11671Saudi Arabia King Abdullah Institute for Nanotechnology King Saud UniversityRiyadh 11451Saudi Arabia

chemodynamic therapy(CDT)based on cascade catalytic nanomedicine has emerged as a promising cancer treatment ***,most of the reported cascade catalytic systems are designed based on symmetric-or co-assembly of multiple catalytic active sites,in which their functions are difficult to perform independently and may interfere with each *** in cascade catalytic system that involves fragile natural-enzymes,the strong oxidation of free-radicals toward natural-enzymes should be carefully considered,and the spatial distribution of the multiple catalytic active sites should be carefully organized to avoid the degradation of the enzyme catalytic ***,a spatially-asymmetric cascade nanocatalyst is developed for enhanced CDT,which is composed by a Fe_(3)O_(4)head and a closely connected mesoporous silica nanorod immobilized with glucose oxidase(mSiO_(2)-GOx).The mSiO_(2)-GOx subunit could effectively deplete glucose in tumor cells,and meanwhile produce a considerable amount of H_(2)O_(2)for subsequent Fenton reaction under the catalysis of Fe_(3)O_(4)subunit in the tumor *** the advantage of the spatial isolation of mSiO_(2)-GOx and Fe_(3)O_(4)subunits,the catalysis of GOx and freeradicals generation occur at different domains of the asymmetric nanocomposite,minimizing the strong oxidation of free-radicals toward the activity of GOx at the other *** addition,direct exposure of Fe_(3)O_(4)subunit without any shelter could further enhance the strong oxidation of free-radicals toward ***,compared with traditional core@shell structure,the long-term stability and efficiency of the asymmetric cascade catalytic for CDT is greatly increased by 138%,thus realizing improved cancer cell killing and tumor restrain efficiency.

关键词： mesoporous nanocatalytic medicine chemodynamic therapy asymmetric nanostructure core@shell

NIR-switchable local hydrogen generation by tandem bimetallic MOFs nanocomposites for enhanced chemodynamic therapy

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Regenerative Biomaterials 2024年第1期3卷 58-68页

作者： Jun Zhong Xiang Zheng Yuan Wen Yuewei Li Jianting Zhang Ranjith Kumar Kankala Shibin Wang Aizheng Chen Institute of Biomaterials and Tissue Engineering Huaqiao UniversityXiamen 361021China Fujian Provincial Key Laboratory of Biochemical Technology Huaqiao UniversityXiamen 361021China Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion Huaqiao UniversityXiamen 361021China

The inadequate quantity of hydrogen peroxide(H_(2)O_(2))in cancer cells promptly results in the constrained success of chemodynamic therapy(CDT).Significant efforts made throughout the years;nevertheless,researchers are still facing the great challenge of designing a CDT agent and securing H_(2)O_(2) supply within the tumor *** this study,taking advantage of H_(2)O_(2) level maintenance mechanism in cancer cells,a nanozyme-based bimetallic metal-organic frameworks(MOFs)tandem reactor is fabricated to elevate intracellular H_(2)O_(2) levels,thereby enhancing *** addition,under nearinfrared excitation,the upconversion nanoparticles(UCNPs)loaded into the MOFs can perform photocatalysis and generate hydrogen,which increases cellular susceptibility to radicals induced from H_(2)O_(2),inhibits cancer cell energy,causes DNA damages and induces tumor cell apoptosis,thus improving CDT therapeutic efficacy *** proposed nanozyme-based bimetallic MOFs-mediated CDT and UCNPs-mediated hydrogen therapy act as combined therapy with high efficacy and low toxicity.

关键词： chemodynamic therapy nanozyme bimetallic MOFs gas therapy

Silica-based nanoarchitecture for an optimal combination of photothermal and chemodynamic therapy functions of Cu2–xS cores with red emitting carbon dots

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 2144-2155页

作者： Alexey Stepanov Svetlana Fedorenko Kirill Kholin Irek Nizameev Alexey Dovzhenko Rustem Zairov Tatiana Gerasimova Alexandra Voloshina Anna Lyubina Guzel Sibgatullina Dmitry Samigullin Asiya Mustafina Arbuzov Institute of Organic and Physical Chemistry FRC Kazan Scientific Center of RASKazan 420088Russia Department of Physics Kazan National Research Technological UniversityKazan 420015Russia Department of Nanotechnology in Electronics Kazan National Research Technical University named after A.N.Tupolev-KAIKazan 420111Russia Kazan(Volga region)Federal University Kazan 420008Russia Kazan Institute of Biochemistry and Biophysics FRC Kazan Scientific Center of RASKazan 420111Russia

This study introduces multifunctional silica nanoparticles that exhibit both high photothermal and chemodynamic therapeutic activities,in addition to *** activity of the silica nanoparticles is derived from their plasmonic properties,which are a result of infusing the silica nanoparticles with multiple Cu2-xS *** infusion process is facilitated by a recoating of the silica nanoparticles with a cationic *** key factors that enable the internal incorporation of the Cu2-xS cores and the external deposition of red-emitting carbon dots are *** Cu2-xS cores within the silica nanoparticles exhibit both self-boosting generation of reactive oxygen species and high photothermal conversion efficacy,which are essential for photothermal and chemodynamic *** silica nanoparticles’small size(no more than 70 nm)and high colloidal stability are prerequisites for their cell *** internalization of the red-emitting silica nanoparticles within cells is visualized using fluorescence microscopy *** chemodynamic activity of the silica nanoparticles is associated with their dark cytotoxicity,and the mechanisms of cell death are evaluated using an apoptotic *** photothermal activity of the silica nanoparticles is demonstrated by significant cell death under near-infrared(1064 nm)irradiation.

关键词： copper sulfide nanoparticles chemodynamic therapy photothermal therapy carbon dots silica nanoparticles

Valence-tailored copper-based nanoparticles for enhanced chemodynamic therapy through prolonged ROS generation and potentiated GSH depletion

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Nano Research 2024年第7期17卷 6342-6352页

作者： Xinyang Li Binbin Ding Jing Li Di Han Hao Chen Jia Tan Qi Meng Pan Zheng Ping’an Ma Jun Lin State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

chemodynamic therapy(CDT),an inventive approach to cancer treatment,exploits innate chemical processes to trigger cell death through the generation of reactive oxygen species(ROS).While offering advantages over conventional treatments,the optimization of CDT efficacy presents challenges stemming from suboptimal catalytic efficiency and the counteractive ROS scavenging effect of intracellular glutathione(GSH).In this study,we aim to address this dual challenge by delving into the role of copper valence states in *** the unique attributes of copper-based nanoparticles,especially zero-valent copper nanoparticles(CuPd NPs),we aim to enhance the therapeutic potential of *** experiments reveal that zero-valent CuPd NPs outperform divalent copper nanoparticles(Ox-CuPd NPs)by displaying superior catalytic performance and sustaining ROS generation through a dual approach integrating peroxidase-like(POD-like)activity and Cu+***,zero-valent NPs exhibit enhanced GSH depletion compared to their divalent counterparts,thereby intensifying CDT and inducing ferroptosis,ultimately resulting in high-efficiency tumor growth *** findings reveal the impact of valences on CDT,providing novel insights for the optimization and design of CDT agents.

关键词： CuPd nanoparticle ferroptosis chemodynamic therapy valance tailoring tumor therapy

Mesothelin targeted nano-system enhanced chemodynamic therapy and tirapazamine chemotherapy via lactate depletion

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Nano Research 2023年第5期16卷 7108-7118页

作者： Guodong Cao Wei Cao Jiawei Zhang Qing Chen Junjie Chen Qiang Chu Qiang Sun Maoming Xiong Bo Chen Xiang Li Department of General Surgery The First Affiliated Hospital of Anhui Medical UniversityHefei 231300China Department of General Surgery The Second Affiliated Hospital of Zhejiang University Medical CollegeHangzhou 310027China State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Jiangsu Key Laboratory of Biological Cancer Cancer instituteXuzhou Medical UniversityXuzhou 221002China Department of surgery the People’s Hospital of Hanshan CountyMa’anshan 238101China

The enhanced permeability and retention(EPR)effect alone is not enough for nanoparticles to reach the *** of active and passive targeting may be an effective drug delivery *** ferric-tannic acid complex nanocapsules(HFe-TA)may effectively degrade and release Fe^(2+) ions,Fe^(2+)ions induce the production of·OH,however,the fenton reaction needs amount of H_(2)O_(2)to enhance chemodynamic *** to their deficiencies,such nanoparticles cannot realize intravenous drug ***,the mesothelin-targeted membrane(MTM)was constructed to realize accurate delivery nano-system,mesothelin antibody was expressed on the 293T cell membrane to prepare a *** oxidase(Lox)was loaded on HFe-TA to obtain Lox@***@HFe-TA was coated with MTM to develop the MTM ***(TPZ)therapy also requires hypoxia *** MTM nanosystem combined with TPZ can significantly kill tumour cells and inhibit metastasis in vivo and in *** also tested the biological safety of the *** this study,we overcame the EPR defects via the MTM nanosystem,which can realize acute targeted delivery to the tumour site,lactate depletion,promoted reactive oxygen species(ROS)induction,enhanced the effect of TPZ,demonstrating a potential synergistic combination of cancer therapy with better efficacy and biosafety.

关键词： mesothelin lactate oxidase tumor metastasis synergetic cancer therapy chemodynamic therapy

Copper-mediated chemodynamic therapy with ultra-low copper consumption by doping cupric ion on cross-linked(R)-(+)-lipoic acid nanoparticles

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Regenerative Biomaterials 2023年第1期10卷 670-677页

作者： Rong Cui Bing Li Chunyan Liao Shiyong Zhang College of Biomedical Engineering National Engineering Research Center for BiomaterialsSichuan UniversityChengdu 610064China Hubei Key Laboratory of Wudang Local Chinese Medicine Research School of Pharmaceutical SciencesHubei University of MedicineShiyan 442000HubeiChina

Cu-mediated chemodynamic therapy(CDT)has attracted prominent attention owing to its advantages of pH independence and high efficiency comparing to Fe-mediated CDT,while the application of Cu-based CDT agents was impeded due to the high copper consumption caused by the metabolism loss of copper and the resultant potential ***,we developed a new copper-mediated CDT agent with extremely low Cu usage by anchoring copper on cross-linked lipoic acid nanoparticles(Cu@cLAs).After endocytosis into tumor cells,the Cu@cLAs were dissociated into LA and dihydrolipoic acid(DHLA)(reduced form of LA)and released Cu^(2+)and Cu+(oxidized form of Cu^(2+)),the two redox couples recycled each other in cells to achieve the efficient killing of cancer cells by delaying metabolic loss and increasing the ROS level of tumor *** self-recycling was confirmed in cells by the sustained high Cu/DHLA content and persistent ROS generation *** antitumor study based on the MCF-7/R nude mice gave the Cu@cLAs a tumor inhibitory rate up to 77.9%at the copper of 0.05 mg kg^(−1),the first dosage reported so far lower than that of normal serum copper(0.83±0.21 mg kg^(−1)).This work provides not only a new promising clinical strategy for the copper excessive use in copper-mediated CDT,but also gives a clue for other metal mediated disease therapies with the high metal consumption.

关键词： chemodynamic therapy copper metabolism (R)-(+)-lipoic acid nanodrug

Mesoporous polydopamine delivery system for intelligent drug release and photothermal-enhanced chemodynamic therapy using MnO_(2) as gatekeeper

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Regenerative Biomaterials 2023年第1期10卷 1566-1576页

作者： Zhaoyang Wang Zekai Li Yuehua Shi Leyong Zeng Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education Chemical Biology Key Laboratory of Hebei ProvinceState Key Laboratory of New Pharmaceutical Preparations and ExcipientsCollege of Chemistry and Materials ScienceHebei UniversityBaoding 071002P.R.China

The non-specific leakage of drugs from nanocarriers seriously weakened the safety and efficacy of chemotherapy,and it was very critical of constructing tumor microenvironment(TME)-responsive delivery nanocarriers,achieving the modulation release of ***,using manganese dioxide(MnO_(2))as gatekeeper,an intelligent nanoplatform based on mesoporous polydopamine(MPDA)was developed to deliver doxorubicin(DOX),by which the DOX release was precisely controlled,and simultaneously the photothermal therapy(PTT)and chemodynamic therapy(CDT)were *** normal physiological environment,the stable MnO_(2)shell effectively avoided the leakage of ***,in TME,the overexpressed glutathione(GSH)degraded MnO_(2)shell,which caused the DOX ***,the photothermal effect of MPDA and the Fenton-like reaction of the generated Mn^(2+)further accelerated the cell ***,the developed MPDA-DOX@MnO_(2)nanoplatform can intelligently modulate the release of DOX,and the combined CDT/PTT/chemotherapy possessed high-safety and high-efficacy against tumors.

关键词： mesoporous polydopamine MnO_(2)gatekeeper chemotherapy photothermal therapy chemodynamic therapy