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Pure drug nano-assemblies: A facile carrier-free nanoplatform for efficient cancer therapy

Acta Pharmaceutica Sinica B 2022年第1期12卷 92-106页

作者： Shuwen Fu Guanting Li Wenli Zang Xinyu Zhou Kexin Shi Yinglei Zhai School of Pharmacy Shenyang Pharmaceutical UniversityShenyang 110016China Department of Pharmaceutics Wuya College of InnovationShenyang Pharmaceutical UniversityShenyang 110016China Department of Periodontology School and Hospital of StomatologyChina Medical UniversityLiaoning Provincial Key Laboratory of Oral DiseaseShenyang 110016China Bio-system Pharmacology Graduate School of MedicineFaculty of MedicineOsaka UniversityOsaka 565-0871Japan Department of Biomedical Engineering School of Medical DeviceShenyang Pharmaceutical UniversityShenyang 110016China

Nanoparticulate drug delivery systems(Nano-DDSs) have emerged as possible solution to the obstacles of anticancer drug delivery. However, the clinical outcomes and translation are restricted by several drawbacks, such as low drug loading, premature drug leakage and carrier-related toxicity.Recently, pure drug nano-assemblies(PDNAs), fabricated by the self-assembly or co-assembly of pure drug molecules, have attracted considerable attention. Their facile and reproducible preparation technique helps to remove the bottleneck of nanomedicines including quality control, scale-up production and clinical translation. Acting as both carriers and cargos, the carrier-free PDNAs have an ultra-high or even100% drug loading. In addition, combination therapies based on PDNAs could possibly address the most intractable problems in cancer treatment, such as tumor metastasis and drug resistance. In the present review, the latest development of PDNAs for cancer treatment is overviewed. First, PDNAs are classified according to the composition of drug molecules, and the assembly mechanisms are discussed. Furthermore, the co-delivery of PDNAs for combination therapies is summarized, with special focus on the improvement of therapeutic outcomes. Finally, future prospects and challenges of PDNAs for efficient cancer therapy are spotlighted.

关键词： Nanotechnology carrier-free Self-assembly Combination therapy Cancer treatment Pure drug Nanomedicine

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carrier-free supramolecular nanomedicines assembled by small-molecule therapeutics for cancer treatment

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Chinese Chemical Letters 2023年第5期34卷 121-131页

作者： Jianhui Zuo Xin Gao Jianru Xiao Yiyun Cheng Department of Thoracic Surgery The First Affiliated Hospital of Anhui Medical UniversityHefei 230022China Shanghai Changzheng Hospital Joint Research Center for Orthopedic Oncology East China Normal UniversityShanghai 200241China Department of Orthopedics Oncology Changzheng HospitalNavy Medical UniversityShanghai 200003China

Nanomedicines have shown great promise in cancer therapy,but are challenged by limited drug loading,safety concerns of drug carriers,and complexity of function integration.Recently,carrier-free nanomedicines produced by supramolecular assembly of small-molecule therapeutic functionalities and their conjugates were proposed to address these issues.These nanomedicines achieve very high drug loading,enhanced tumor accumulation and improved therapeutic efficiency,and avoid carrier-related safety problems.In this review article,the applications of these nanomedicines in chemotherapy,photodynamic therapy,photothermal therapy as well as combination therapies will be reviewed.The concept of nanomedicine design and mechanism of supramolecular assembly will be discussed.Finally,future perspectives of carrier-free supramolecular nanomedicines for cancer therapy will be highlighted.

关键词： Nanomedicine carrier-free Cancer therapy Supramolecular assembly Combination therapy

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Ce6 nanoassemblies:Molecular mechanism and strategies for combinational anticancer therapy Special Collection:Aggregation-Induced Processes and Functions

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Aggregate 2024年第1期5卷 130-147页

作者： Yuwei Liu Shuting Xu Qingyang Lyu Yi Huang Weiping Wang State Key Laboratory of Pharmaceutical Biotechnology The University of Hong KongHong KongChina Department of Pharmacology and Pharmacy Li Ka Shing Faculty of MedicineThe University of Hong KongHong KongChina Laboratory of Molecular Engineering and Nanomedicine Dr.Li Dak-Sum Research CentreThe University of Hong KongHong KongChina

Nowadays,cancer has become the leading cause of death worldwide,driving the need for effective therapeutics to improve patient prognosis.Photodynamic therapy(PDT)has been widely applied as an antitumor modality,owing to its minimal invasiveness,localized tumor damage,and high safety profile.However,its efficacy is limited by poor stability of photosensitizers,inadequate tumor accumulation,and a complex tumor microenvironment.To overcome these challenges,extensive endeavors have been made to explore the co-assembly of the widely used photosensitizer chlorin e6(Ce6)with various functional small molecules to enhance pharmacodynamic activity.This review provides a comprehensive overview of current studies on Ce6-based nanoparticles for effective PDT and precise delivery of functional molecules.The self-assembly mechanism will be discussed in detail,with a focus on potential strategies for combinational therapy with PDT.

关键词： cancer treatment carrier-free chlorin e6(Ce6) light nanomedicine photodynamic therapy(PDT) selfassembly

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carrier-free Deferoxamine Nanoparticles against Iron Overload in Brain

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CCS Chemistry 2023年第1期5卷 257-270页

作者： Fang Zhu Jian Zhong Junfei Hu Peng Yang Jianhua Zhang Minghua Zhang Yiwen Li Zhipeng Gu College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengduSichuan 610065 State Key Laboratory of Biotherapy and Cancer West China HospitalSichuan University and Collaborative Innovation CenterChengdu 610041

Although considerable progress has been achieved in treating iron-overload diseases with deferoxamine(DFO)-based biomaterials,high DFO loading and multifunctional integration in one system are still grand challenges.Herein,a series of carrier-free,high DFO-loading(∼80%),uniform spherical nanoparticles(NPs)assisted by polyphenols have been facilely developed with both efficient iron and reactive oxygen species-scavenging properties.Interestingly,those DFO-based NPs have demonstrated excellent scavenging performance in iron-overloaded cell model and energetically exhibited brain cell protection in vivo in intracerebral hemorrhage animal models.This study could provide a promising strategy to significantly improve the curative effect of DFO delivery systems for iron-overload diseases.

关键词： carrier-free deferoxamine nanoparticles iron scavenging reactive oxygen species scavenging

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Erythrocyte membrane-camouflaged carrier-free nanoassembly of FRET photosensitizer pairs with high therapeutic efficiency and high security for programmed cancer synergistic phototherapy

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Bioactive Materials 2021年第8期6卷 2291-2302页

作者： Xuanbo Zhang Jianchen Xiong Kaiyuan Wang Han Yu Bingjun Sun Hao Ye Zhiqiang Zhao Ning Wang Yuequan Wang Shenwu Zhang Wutong Zhao Haotian Zhang Zhonggui He Cong Luo Jin Sun Department of Pharmaceutics Wuya College of InnovationShenyang Pharmaceutical UniversityShenyangLiaoning110016PR China School of Life Science and Biopharmaceutics Shenyang Pharmaceutical UniversityShenyang110016PR China

Phototherapy has been intensively investigated as a non-invasive cancer treatment option.However,its clinical translation is still impeded by unsatisfactory therapeutic efficacy and severe phototoxicity.To achieve high therapeutic efficiency and high security,a nanoassembly of Forster Resonance Energy Transfer(FRET)photosensitizer pairs is developed on basis of dual-mode photosensitizer co-loading and photocaging strategy.For proof-of-concept,an erythrocyte-camouflaged FRET pair co-assembly of chlorine e6(Ce6,FRET donor)and 1,1′-dioctadecyl-3,3,3′,3′-tetramethylindotricarbocyanine iodide(DiR,FRET acceptor)is investigated for breast cancer treatment.Notably,Ce6 in the nanoassemby is quenched by DiR and could be unlocked for photodynamic therapy(PDT)only when DiR is photobleached by 808-nm laser.As a result,Ce6-caused phototoxicity could be well controlled.Under cascaded laser irradiation(808-660 nm),tumor-localizing temperature rise following laser irradiation on DiR not only induces tumor cell apoptosis but also facilitates the tumor penetration of NPs,relieves tumor hypoxia,and promotes the PDT efficacy of Ce6.Such FRET pair-based nanoassembly provides a new strategy for developing multimodal phototherapy nanomedicines with high efficiency and good security.

关键词： FRET pair carrier-free Nanoassembly Erythrocyte membrane-camouflaged Programmed synergistic phototherapy

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Self-assembling, pH-responsive nanoflowers for inhibiting PAD4 and neutrophil extracellular trap formation and improving the tumor immune microenvironment

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Acta Pharmaceutica Sinica B 2022年第5期12卷 2592-2608页

作者： Di Zhu Yu Lu Lin Gui Wenjing Wang Xi Hu Su Chen Yanming Wang Yuji Wang Department of Medicinal Chemistry College of Pharmaceutical Sciences of Capital Medical UniversityBeijing 100069China Beijing Area Major Laboratory of Peptide and Small Molecular Drugs Engineering Research Center of Endogenous Prophylactic of Ministry of Education of ChinaBeijing Laboratory of Biomedical MaterialsBeijing 100069China Beijing Institute of Hepatology Beijing Youan HospitalCapital Medical UniversityBeijing 100069China Quantum Design China Ltd. Universal Business ParkBeijing 100015China Laboratory of Biomaterials and Biomechanics Beijing Key Laboratory of Tooth Regeneration and Function ReconstructionSchool of StomatologyCapital Medical UniversityBeijing 100050China School of Life Sciences Henan UniversityKaifeng 475004China

Self-assembling carrier-free nanodrugs are attractive agents because they accumulate at tumor by an enhanced permeability and retention(EPR) effect without introduction of inactive substances,and some nanodrugs can alter the immune environment. We synthesized a peptidyl arginine deiminase 4(PAD4) molecular inhibitor, ZD-E-1 M. It could self-assembled into nanodrug ZD-E-1. Using confocal laser scanning microscopy, we observed its cellular colocalization, PAD4 activity and neutrophil extracellular traps(NETs) formation. The populations of immune cells and expression of immune-related proteins were determined by single-cell mass cytometry. ZD-E-1 formed nanoflowers in an acidic environment, whereas it formed nanospheres at pH 7.4. Accumulation of ZD-E-1 at tumor was pHresponsive because of its pH-dependent differences in the size and shape. It could enter the nucleus and bind to PAD4 to prolong the intracellular retention time. In mice, ZD-E-1 inhibited tumor growth and metastasis by inhibiting PAD4 activity and NETs formation. Besides, ZD-E-1 could regulate the ratio of immune cells in LLC tumor-bearing mice. Immunosuppressive proteins like LAG3 were suppressed,while IFN-γ and TNF-a as stimulators of tumor immune response were upregulated. Overall, ZD-E-1 is a self-assembling carrier-free nanodrug that responds to pH, inhibits PAD4 activity, blocks neutrophil extracellular traps formation, and improves the tumor immune microenvironment.

关键词： pH-Response Self-assembly carrier-free Nanoflowers Neutrophil extracellular traps Single-cell mass cytometry Tumor immune microenvironment Lymphocyte activation gene-3

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Secret Data-Driven carrier-free Secret Sharing Scheme Based on Error Correction Blocks of QR Codes

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国际计算机前沿大会会议论文集 2017年第1期 56-57页

作者： Song Wan Yuliang Lu Xuehu Yan Hanlin Liu Longdan Tan Hefei Electronic Engineering Institute Hefei 230037China

In this paper,a novel secret data-driven carrier-free(semi structural formula)visual secret sharing(VSS)scheme with(2,2)threshold based on the error correction blocks of QR codes is investigated.The proposed scheme is to search two QR codes that altered to satisfy the secret sharing modules in the error correction mechanism from the large datasets of QR codes according to the secret image,which is to embed the secret image into QR codes based on carrier-free secret sharing.The size of secret image is the same or closest with the region from the coordinate of(7,7)to the lower right corner of QR codes.In this way,we can find the QR codes combination of embedding secret information maximization with secret data-driven based on Big data search.Each output share is a valid QR code which can be decoded correctly utilizing a QR code reader and it may reduce the likelihood of attracting the attention of potential attackers.The proposed scheme can reveal secret image visually with the abilities of stacking and XOR decryptions.The secret image can be recovered by human visual system(HVS)without any computation based on stacking.On the other hand,if the light-weight computation device is available,the secret image can be lossless revealed based on XOR operation.In addition,QR codes could assist alignment for VSS recovery.The experimental results show the effectiveness of our scheme.

关键词： Visual secret sharing QR code Error correction blocks carrier-free Big data Data-driven Multiple decryptions

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Elaborately engineering of a dual-drug co-assembled nanomedicine for boosting immunogenic cell death and enhancing triple negative breast cancer treatment

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Asian Journal of Pharmaceutical Sciences 2022年第3期17卷 412-424页

作者： Chen Wang Han Yu Xiaohong Yang Xuanbo Zhang Yuequan Wang Tianrui Gu Shenwu Zhang Cong Luo Shenyang Pharmaceutical University Shenyang 110016China

Pure drug-assembled nanosystem provides a facile and promising solution for simple manufacturing of nanodrugs,whereas a lack of understanding of the underlying assembly mechanism and the inefficient and uncontrollable drug release still limits the development and application of this technology.Here,a simple and practical nanoassembly of DOX and DiR is constructed on basis of their co-assembly characteristics.Multiple interaction forces are found to drive the co-assembly process.Moreover,DOX release from the nanoassembly can bewell controlled by the acidic tumormicroenvironment and laser irradiation,resulting in favorable delivery efficiency of DiR and DOX in vitro and in vivo.As expected,the nanoassembly with high therapeutic safety completely eradicated the mice triple negative breast cancer cells(4T1)on BALB/c mice,owing to synergistic chemo-photothermal therapy.More interestingly,DiR and DOX synergistically induce immunogenic cell death(ICD)of tumor cells after treatment,enabling the mice to acquire immune memory against tumor growth and recurrence.Such a facile nanoassembly technique provides a novelmultimodal cancer treatment platform of chemotherapy/phototherapy/immunotherapy.

关键词： carrier-free Pure drug co-assembly Immune activation Synergistic chemo-photothermal therapy

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Evolution from small molecule to nano-drug delivery systems:An emerging approach for cancer therapy of ursolic acid

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Asian Journal of Pharmaceutical Sciences 2020年第6期15卷 685-700页

作者： Jingwei Shao Yifan Fang Ruirui Zhao Fangmin Chen Mingyue Yang Jiali Jiang Zixuan Chen Xiaotian Yuan Lee Jia Cancer Metastasis Alert and Prevention Center and Fujian Provincial Key Laboratory of Cancer Metastasis Chemoprevention and ChemotherapyCollege of ChemistryFuzhou UniversityFuzhou 350116China Marine Drug R&D Center Institute of OceanographyMinjiang UniversityFuzhou 350108China

Ursolic acid(UA),a natural pentacyclic triterpenoid,possesses widespread biological and pharmacological activities.However,drawbacks such as low bioavailability,poor targeting and rapid metabolism greatly hinder its further clinical application.Recently,with the development of nanotechnology,various UA nanosystems have emerged as promising strategies for effective cancer therapy.This article reviews various types of UA-based nanodelivery systems,primarily with emphasis placed on novel UA-based carrier-free nanodrugs,which are considered to be innovative methods for cancer therapy.Moreover,this review presents carrier-free nano-drugs that co-assembled of UA and photosensitizers that displayed synergistic antitumor performance.Finally,the article also describes the development and challenges of UA nanosystems for future research in this field.Overall,the information presented in this review will provide new insight into the rational utilization of nano-drugs in cancer therapy.

关键词： Ursolic acid Nanosytems carrier-free Photosensitizer Anticancer

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Redox-responsive micelles integrating catalytic nanomedicine and selective chemotherapy for effective tumor treatment

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Chinese Chemical Letters 2021年第10期32卷 3076-3082页

作者： Ronghua Jin Zhongning Liu Tao Liu Pingyun Yuan Yongkang Bai Xin Chen School of Chemical Engineering and Technology Shaanxi Key Laboratory of Energy Chemical Process IntensificationInstitute of Polymer Science in Chemical EngineeringXi'an Jiao Tong UniversityXi’an 710049China Pharmaceutical College Guangxi Medical UniversityBeijing 100081China Department of Prosthodontics Peking University School and Hospital of StomatologyNational Engineering Laboratory for Digital and Material Technology of StomatologyBeijing Key Laboratory of Digital StomatologyNanning 530021China

Chemotherapy is one of the most conventional modalities for cancer therapy.However,the high multidrug resistance of tumor cells still limited the clinical application of current chemotherapy.Considering the ability of nitric oxide(NO) to modulate potent P-glycoprotein to inhibit multi-drug resistance,a synergistic methodology combining chemotherapy and sustained NO generation is an ideal way to further promote the chemotherapy.Herein,a multi-functional micelle with tumor-selective chemotherapy driven by redox-triggered doxorubicin(DOX) release and drug resistance inhibition based on intracellular NO generation was fabricated for effective tumor treatment.The micelle consists of DOX as core,arginine/glucose oxidase(Arg/GOx) as shell and redox-responsive disulfide bond as a linker,which is denoted as micelle-DOX-Arg-GOx.The Arg serves as the biological precursor of nitric oxide for inhibition of multi-drug resistance to promote chemotherapy and GOx catalyzes glucose to produce hydrogen peroxide(H_(2) O_(2)) for increasing the generation of NO.Moreover,the glucose supply could be simultaneously blocked by the catalytic process,which further enhanced therapeutic efficiency.This micelle requests a tumor-specific microenvironment(a considerable amount of GSH) to perform synergistic therapeutics including chemotherapy,starvation therapy(catalytic medicine),and gas therapy for tumor treatment,which resulted in significant cytotoxicity to tumor tissue.

关键词： Chemotherapy Gas therapy Starvation therapy carrier-free Tumor treatment

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