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tumor microenvironment-activatable neuropeptide-drug conjugates enhanced tumor penetration and inhibition via multiple delivery pathways and calcium deposition

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Chinese Chemical Letters 2024年第4期35卷 292-297页

作者： Yi Cao Xiaojiao Ge Yuanyuan Wei Lulu He Aiguo Wu Juan Li Ningbo Key Laboratory of Biomedical Imaging Probe Materials and Technology Zhejiang International Cooperation Base of Biomedical Materials Technology and ApplicationChinese Academy of Sciences(CAS)Key Laboratory of Magnetic Materials and DevicesNingbo Cixi Institute of Biomedical EngineeringZhejiang Engineering Research Center for Biomedical MaterialsNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China University of Chinese Academy of Sciences Beijing 100049China Advanced Energy Science and Technology Guangdong Laboratory Huizhou 516000China

Peptide-drug conjugates have achieved considerable development and application as a novel strategy for targeted delivery of anticancer drugs. Bioactive peptides induced calcium deposition can irreversibly assist inhibition of tumors. However, active regulation of calcium level through signal transduction of bioactive substances has not been reported yet. In this study, novel neuropeptide-doxorubicin conjugates(NP-DOX) with lysosome-specific acid response were described for neuropeptide Y_1 receptor(Y_1R)-overexpressed triple-negative breast cancer. The delivery mechanism of NP-DOX was clarified that diverse pathways were involved, including intracellular and intercellular transport. Importantly, up-regulation of Y_1 R-mediated intracellular calcium level via second messenger inositol triphosphate was presented in NP-DOX treated MDA-MB-231 cells. In vivo antitumor efficacy demonstrated that NP-DOX showed less organ toxicity and enhanced tumor inhibition benefited from its controlled release and Y_1R-mediated calcium deposition, compared with free DOX. This bioconjugate is a proof-of-concept confirming that neuropeptide-mediated control of signaling responses in neuropeptide-drug conjugates enables great potential for further applications in tumor chemotherapy.

关键词： Neuropeptide-drug conjugate tumor penetration Calcium deposition tumor inhibition Triple-negative breast cancer

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Self-assembly nanomicelle-microneedle patches with enhanced tumor penetration for superior chemo-photothermal therapy

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Nano Research 2022年第3期15卷 2335-2346页

作者： Ying Sun Minglong Chen Dan Yang Wanbing Qin Guilan Quan Chuanbin Wu Xin Pan School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou 510006China College of Pharmacy Jinan UniversityGuangzhou 510632China Jieyang Affiliated Hospital Sun Yat-Sen UniversityGuangzhou 522091China Physical Sciences at the Microscale Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Nanomedicine with high specificity has been a promising tool for cancer diagnosis and therapy.However,the successful application of nanoparticle-based superficial cancer therapy is severely hindered by restricted deep tumor tissue accumulation and penetration.Herein,a self-assembly nanomicelle dissolving microneedle(DMN)patch according to the“nano in micro”strategy was conducted to co-deliver a first-line chemotherapeutic agent paclitaxel(PTX),and a photosensitizer IR780(PTX/IR780-NMs@DMNs)for chemo-photothermal synergetic melanoma therapy.Upon direct insertion into the tumor site,DMNs created a regular and multipoint three-dimensional drug depot to maximize the tumor accumulation.Accompanied by the DMN dissolution,the composition of the needle matrixes self-assembled into nanomicelles,which could efficiently penetrate deep tumor tissue.Upon laser irradiation,the nanomicelles could not only ablate tumor cells directly by photothermal conversion but also trigger PTX release to induce tumor cell apoptosis.In vivo results showed that compared with intravenous injection,IR780 delivered by PTX/IR780-NMs@DMNs was almost completely accumulated at the tumor site.The antitumor results revealed that the PTX/IR780-NMs@DMNs could effectively eliminate tumors with an 88%curable rate without any damage to normal tissues.This work provides a versatile and generalizable framework for designing self-assembly DMN-mediated combination therapy to fight against superficial cancer.

关键词： dissolving microneedle tumor penetration nanomicelle superficial tumor chemo-photothermal therapy

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Sequentially responsive size reduction and drug release of core-satellite nanoparticles to enhance tumor penetration and effective tumor suppression

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Chinese Chemical Letters 2023年第5期34卷 489-493页

作者： Jiayi Sun Jingyang Li Xi Li Lu Yang Yitong Liu Huile Gao Li Xiang State Key Laboratory of Southwestern Chinese Medicine Resources Innovative Institute of Chinese Medicine and PharmacyChengdu University of Traditional Chinese MedicineChengdu 611137China Public Health Clinical Center of Chengdu Chengdu 610061China The Third Affiliated Hospital of Chengdu University of TCM/Chengdu Pidu District Hospital of Traditional Chinese Medicine Chengdu 611730China West China School of Pharmacy Sichuan UniversityChengdu 610041China

Poor tumor accumulation remains a serious challenge for nanomedicines to achieve ideal antitumor outcomes.The different size preferences for systematic circulation,tumor retention and deep permeation have attracted great attention when designing antineoplastic nano-delivery system.Herein,we developed a nano-system which can shrink its size in tumor microenvironment to achieve better tumor retention and penetration.In this work,the cationic bovine serum albumin-protected,doxorubicin-loaded gold nanoclusters(CAuNC-DOX)and amino-functionalized mesoporous silica nanoparticles(MSN)are connected by Fe^(2+)and are further coated with hyaluronic acid(HA)to obtain a core-satellite MSN-Fe-CAuNCDOX@HA nano system(MFADH).When reaching the tumor site,the HA shell,which endows the system with both good biocompatibility and preferable tumor targeting ability,was disintegrated,followed by acid-stimulated release of small-sized pharmacological unit—CAuNC-DOX for further tumor penetration.As demonstrated in both in vitro and in vivo results,MFADH showed excellent antitumor effect,providing a proof of concept for the feasibility of shrinkable nanoplatforms in tumor treatment.

关键词： Size reducible tumor penetration Core-satellite structure Mesoporous silica nanoparticles Gold nanoclusters Experimental techniques

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A Magnetocatalytic Propelled Cobalt-Platinum@Graphene Navigator for Enhanced tumor penetration and Theranostics

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CCS Chemistry 2022年第7期4卷 2382-2395页

作者： Liang Zhang Qian Dong Hui Zhang Jieqiong Xu Shen Wang Lufeng Zhang Wentao Tang Zhaoqian Li Xin Xia Xinqi Cai Shengkai Li Ruizi Peng Zhengyu Deng Michael JDonovan Long Chen Zhuo Chen Weihong Tan 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 UniversityChangshaHunan 410082 Faculty of Science and Technology University of MacaoTaipaMacao 999078 The Cancer Hospital of the University of Chinese Academy of Sciences(Zhejiang Cancer Hospital) Institute of Basic Medicine and Cancer(IBMC)Chinese Academy of SciencesHangzhouZhejiang 310022

Complex biological environments and multiple physiological barriers significantly impede efficient accumulation and penetration of nanomaterials within tumor tissue for therapy.In situ energy conversion of nanomotors features autonomous movements and improves cancer treatment.However,one of the key challenges is to prepare nanomotors with an adequately small size,good biocompatibility,and precise positioning.Herein,we demonstrate a simple,ultrasmall,versatile,and real-time motion guidance strategy for magnetocatalytic CoPt@graphene navigators(MCGNs)that can enable highly efficient propulsion in the presence of H_(2)O_(2) or magnetic actuation.MCGNs act as highly diffusive delivery vehicles to promote tumor tissue targeting,and the amount of drug in the tumor was three times than without navigation.By engaging movements powered through in situ energy conversion,MCGNs gain considerable propulsion to penetrate a cell’s membrane and enhance intracellular delivery.

关键词： magnetocatalytic propelled nanomotors navigator tumor penetration photothermal therapy tumor theranostics

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Soft Mesoporous Organosilica Nanoplatforms Improve Blood Circulation,tumor Accumulation/penetration,and Photodynamic Efficacy

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Nano-Micro Letters 2020年第10期12卷 205-223页

作者： Xin Peng Kun Chen Wanhua Liu Xiongfeng Cao Mengru Wang Jun Tao Ying Tian Lei Bao Guangming Lu Zhaogang Teng Jiangsu Key Laboratory of Molecular and Functional Imaging Department of RadiologyZhongda HospitalSchool of MedicineSoutheast UniversityNanjing 210009JiangsuPeople’s Republic of China Department of Medical Imaging Jinling HospitalSchool of MedicineNanjing UniversityNanjing 210002People’s Republic of China Key Laboratory for Organic Electronics and Information Displays Jiangsu Key Laboratory for BiosensorsInstitute of Advanced MaterialsJiangsu National Synergetic Innovation Centre for Advanced MaterialsNanjing University of Posts and TelecommunicationsNanjing 210023People’s Republic of China Affiliated Hospital of Jiangsu University Jiangsu UniversityZhenjiang 212001People’s Republic of China Soft Matter and Interface Group School of EngineeringRMIT UniversityMelbourneVIC 3000Australia

To date,the ability of nanoplatforms to achieve excellent therapeutic responses is hindered by short blood circulation and limited tumor accumulation/penetration.Herein,a soft mesoporous organosilica nanoplatform modified with hyaluronic acid and cyanine 5.5 are prepared,denoted SMONs-HA-Cy5.5,and comparative studies between SMONs-HA-Cy5.5(24.2 MPa)and stiff counterparts(79.2 MPa)are conducted.Results indicate that,apart from exhibiting a twofold increase in tumor cellular uptake,the soft nanoplatforms also display a remarkable pharmacokinetic advantage,resulting in considerably improved tumor accumulation.Moreover,SMONs-HA-Cy5.5 exhibits a significantly higher tumor penetration,achieving 30-μm deeper tissue permeability in multicellular spheroids relative to the stiff counterparts.Results further reveal that the soft nanoplatforms have an easier extravasation from the tumor vessels,diffuse farther in the dense extracellular matrix,and reach deeper tumor tissues compared to the stiff ones.Specifically,the soft nanoplatforms generate a 16-fold improvement(43 vs.2.72μm)in diffusion distance in tumor parenchyma.Based on the significantly improved blood circulation and tumor accumulation/penetration,a soft therapeutic nanoplatform is constructed by loading photosensitizer chlorin e6 in SMONs-HA-Cy5.5.The resulting nanoplatform exhibits considerably higher therapeutic efficacy on tumors compared to the stiff ones.

关键词： Mesoporous organosilica Soft nanoplatform Long circulation tumor accumulation tumor penetration

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Self-assembled FeS-based cascade bioreactor with enhanced tumor penetration and synergistic treatments to trigger robust cancer immunotherapy

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Acta Pharmaceutica Sinica B 2021年第10期11卷 3244-3261页

作者： Hao Ren Jiahui Yong Qingqing Yang Zhen Yang Zhangya Liu Yan Xu Hao Wang Xing Jiang Wenjun Miao Xueming Li School of Pharmaceutical Science Nanjing Tech UniversityNanjing 211816China School of Nursing Nanjing University of Chinese MedicineNanjing 210023China

Major challenges for cancer treatment are how to effectively eliminate primary tumor and sufficiently induce immunogenic cell death(ICD)to provoke a robust immune response for metastasis control.Here,a self-assembled cascade bioreactor was developed to improve cancer treatment with enhanced tumor penetration and synergistic therapy of starvation,chemodynamic(CDT)and photothermal therapy.Ultrasmall Fe S-GOx nanodots were synthesized with glucose oxidase(GOx)as template and induced by paclitaxel(PTX)to form self-assembling Fe S-GOx@PTX(FGP)via hydrophobic interaction.After accumulated at tumor sites,FGP disassembles to smaller Fe S-GOx for enhanced deep tumor penetration.GOx maintains high enzymatic activity to catalyze glucose with assistant of oxygen to generate hydrogen peroxide(H2O2)as starvation therapy.Fenton reaction involving the regenerated H_(2)O_(2) in turn produced more hydroxyl radicals for enhanced CDT.Following near-infrared laser at 808 nm,FGPs displayed pronounced tumor inhibition in vitro and in vivo by the combination therapy.The consequent increased exposure to calreticulin amplified ICD and promoted dendritic cells maturation.In combination with anti-CTLA4 checkpoint blockade,FGP can absolutely eliminate primary tumor and avidly inhibit distant tumors due to the enhanced intratumoral infiltration of cytotoxic T lymphocytes.Our work presents a promising strategy for primary tumor and metastasis inhibition.

关键词： Fe S-based cascade bioreactor Glucose oxidase tumor penetration Synergistic therapy ICD amplifier Cancer immunotherapy Metastasis inhibition

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The progress and perspective of strategies to improve tumor penetration of nanomedicines

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Chinese Chemical Letters 2021年第4期32卷 1341-1347页

作者： Jiang Hu Xinwei Yuan Fei Wang Huile Gao Xilin Liu Wei Zhang Department of Orthopedics Sichuan Provincial People's Hospital&Sichuan Academy of Medical Sciences&Affiliated Hospital of University of Electronic Science and TechnologyChengdu 610072China Key Laboratory of Drug Targeting and Drug Delivery System of the Education Ministry Sichuan Engineering Laboratory for Plant-Sourced Drug and Sichuan Research Center for Drug Precision Industrial TechnologyWest China School of Pharmacy Sichuan UniversityChengdu 610041China

tumor penetration is important for effectively tumor targeting drug delivery.Recently,many researches are published to overcome the barriers that restrict tumor penetration and improve drug delivery efficiency.In the mini review,we first analyzed the barriers influence the tumor penetration,including tumor microenvironment barriers,nanoparticle properties,and interaction barriers between tumor and nanoparticles.To overcome the barrier,several strategies are developed,including modulating tumor microenvironment,changing particle size,transcytosis enabled tumor penetration,cell penetrating peptide modification and overcoming binding site barrier,which could effectively improve tumor penetration,and finally enhance tumor treatment outcome.

关键词： tumor penetration tumor microenvironment Size changeable Cell penetrating peptide Nanoparticles

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Two-dimensional LDH nanodisks modified with hyaluronidase enable enhanced tumor penetration and augmented chemotherapy

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Science China Chemistry 2021年第5期64卷 817-826页

作者： Gaoming Li Yu Fan Lizhou Lin Rong Wu Mingwu Shen Xiangyang Shi State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of ChemistryChemical Engineering and BiotechnologyDonghua UniversityShanghai 201620China Department of Ultrasound Shanghai General HospitalShanghai Jiao Tong University School of MedicineShanghai 200080China

The condensed tumor extracellular matrix(ECM)consisting of cross-linked hyaluronic acid(HA)is one of the key factors that result in the aberrant tumor microenvironment and severely impair drug delivery and tumor penetration.Herein,we report a simple design of a hyaluronidase(HAase)-modified layered double hydroxide(LDH)nanoplatform loaded with anticancer drug doxorubicin(DOX)for enhanced tumor penetration and augmented chemotherapy.In our approach,LDH nanodisks were synthesized via a co-precipitation method,modified with HAase by electrostatic attraction,and finally physically loaded with DOX.The formulated DOX/LDH-HAase complexes show a high DOX loading percentage of 34.2%with good colloidal stability,retain 86.1%of the enzyme activity,and release DOX in a pH-responsive manner having a faster release rate under slightly acidic tumor microenvironment than that under a physiological condition.With the catalytic activity of HAase to digest the HA nearby the cancer cells,the developed DOX/LDH-HAase complexes enable more significant uptake by cancer cells and penetration in 3-dimensional tumor spheroids than enzyme-free DOX/LDH complexes,thus displaying much better antitumor efficacy in vitro than the latter.The more significant tumor penetration and inhibition of the DOX/LDH-HAase complexes than that of the DOX/LDH complexes was further demonstrated by in vivo tumor imaging and therapeutic activity assessments.Our study suggests a unique nanomedicine platform combined with both anticancer drug and enzyme for improved tumor penetration and chemotherapy,which is promising for effective chemotherapy of different types of stroma-rich tumors.

关键词： pancreatic cancer layered double hydroxide hyaluronidase tumor penetration chemotherapy

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Mechanism investigation of tumor microenvironment response multistage nanoparticles for deep tumor penetration

Mechanism investigation of tumor microenvironment response m...

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2018年第十二届中国药物制剂大会

作者：陈恩蕊 Jialing DAI Shangcong HAN Jie CAO Yan LIANG Yong SUN School of Pharmacy Qingdao University

Hyaluronic acid（HA） is the main component of the extracellular matrix（ECM） and the overexpression of HA in tumors contributes to a gel-like extracellular matrix that increase the interstitial fluid pressure（IFP）, thus hindered the deep tumor penetration of nanoparticles. To enhance the poor tumor penetration and reduce the IFP, we developed a tumor microenvironment response multistage drug delivery system, which was formed via electrostatic interaction with cationic drug-loaded nanoparticles（m PEG-PDPA-PG-DOX） and hyaluronidase（HAase） that could degrade HA. We firstly formed doxorubicin（DOX）-uploaded m PEGPDPA-PG nanoparticles（NPs-DOX） by self-assembling. Due to the protonation of tertiary amine groups of PDPA segment in acid environment like endosomes or lysosomes, m PEG-PDPA-PG could enhance the lysosome escape and the intracellular release of DOX. Dynamic light scattering（DLS） of NPs-DOX showed an average size of 95 nm, while the size measured with transmission electron microscopy（TEM） was approximately 30 nm. Compared with larger nanoparticles with size of 200 nm, this small particle size nanoparticle is favorable to reach the deep region of tumor. Then, the effect of HAase treatment on nanoparticles penetration after electrostatic interaction was systematically assessed in tumor spheroid and solid tumors. The confocal images showed that NPs-DOX was located at the edge of tumor spheroid, while the fluorescence of NPs-DOX/HAase distributed more extensively and penetrated much deeper in the distance. Besides, treatment of spheroids with low concentration of HAase resulted in a slight loosening of cells at the outer spheroid perimeter, whereas treatment with high concentration of hyaluronidase significantly affected spheroid architecture. In the future, we will further confirm NPs-DOX/HAase will significantly degrade majority of tumor HA and reduce IFP by peritumoral injection.

关键词： hyaluronidase tumor penetration ECM IFP nanoparticles

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Priming the tumor microenvironment by a cancer-associated fibroblasts targeted liposome for improving deep tumor penetration of targeted nanovesicles and combined therapy

Priming the tumor microenvironment by a cancer-associated fi...

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2015年中国药学大会暨第十五届中国药师周

作者： Binlong Chen Wenbing Dai Bing He Hua Zhang Xueqing Wang Qiang Zhang Beijing Key Laboratory of Molecular Pharmaceutics and New Drug Delivery Systems School of Pharmaceutical Sciences Peking University State Key Laboratory of Natural and Biomimetic Drugs

Inefficient tumor penetration and drug resistance both related to tumor microenvironment are major barriers for traditional tumor-targeted chemotherapeutic drug delivery systems. Cancer-associated fibroblasts（CAFs） play a vitally important role during tumor initiation, angiogenesis, progression and metastasis. Navitoclax（Nav） can specifically induce apoptosis in CAFs, which are abundant in the stroma of solid tumor and the main source of collagen. Both CAFs and collagen can raise the interstitial fluid pressure（IFP） in tumor, which presents a transport barrier that restricts nanoparticle penetration into the deep of tumor, thereby limiting the efficacy of nano-drug delivery vehicles for cancer therapy. We have developed a novel tumor stroma-targeted nanovehicle, Nav-loaded nanoliposomes modified with peptide FH（FH-SSL-Nav）, which specifically binds to tenascin C, a protein mainly expressed by CAFs, to target and specifically eradicate CAFs, which have extensive cross-talk with cancer cells and play a pivotal role on maintaining tumor microenvironment beneficial to tumor growth and resistance to cancer therapies. Several experiments were performed to evaluate CAFs selective apoptosis, targeting and eradicating. Compared with SSL-Nav, FH-SSL-Nav achieved higher cellular uptake by flow cytometry and confocal microscopy, and exhibited stronger cytotoxicity in vitro. The in vivo tumor stroma targeting effect was further confirmed by near infrared imaging. Based on its primary effect of eradicating CAFs, FH-SSL-Nav exhibited excellent tumor microenvironment modulation including downregulation ECM deposition, decreasing interstitial fluid pressure（IFP） and facilitating blood perfusion. As a result, with physical barrier destroyed, more nanovesicles penetrated deep into tumor. In antitumor studies, it was proved again that FH-SSL-Nav greatly improved the tumor suppression of liposomal DOX with low toxicity. Thus, this study may provide a novel strategy for combined therapeutic regimens based on tumor microenvironment pri

关键词： Cancer-associated fibroblasts tumor microenvironment Navitoclax, Liposomal doxorubicin Combination therapy tumor penetration

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