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Self-fueling ferroptosis-inducing microreactors based on p H-responsive Lipiodol Pickering emulsions enable transarterial ferro-embolization therapy

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National Science Review 2024年第1期11卷 74-85页

作者： Chunjie Wang Lei Zhang Zhijuan Yang dongxu Zhao Zheng Deng Jialu Xu Yumin Wu Yu Hao ziliang dong Liangzhu Feng Zhuang Liu Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Center of Interventional Radiology & Vascular Surgery Department of Radiology Zhongda Hospital Medical School Southeast University Department of Interventional Radiology The First Afflliated Hospital of Soochow University

Lipiodol chemotherapeutic emulsions remain one of the main choices for the treatment of unresectable hepatocellular carcinoma(HCC) via transarterial chemoembolization(TACE). However, the limited stability of Lipiodol chemotherapeutic emulsions would lead to rapid drug diffusion, which would reduce the therapeutic benefit and cause systemic toxicity of administrated chemotherapeutics. Therefore, the development of enhanced Lipiodol-based formulations is of great significance to enable effective and safe TACE treatment. Herein, a stable water-in-oil Lipiodol Pickering emulsion(LPE) stabilized by pH-dissociable calcium carbonate nanoparticles and hemin is prepared and utilized for efficient encapsulation of lipoxygenase(LOX). The obtained LOX-loaded CaCO3&hemin-stabilized LPE(LHCa-LPE) showing greatly improved emulsion stability could work as a pH-responsive and self-fueling microreactor to convert polyunsaturated fatty acids(PUFAs), a main component of Lipiodol, to cytotoxic lipid radicals through the cascading catalytic reaction driven by LOX and hemin, thus inducing ferroptosis of cancer cells. As a result, such LHCa-LPE upon transcatheter embolization can effectively suppress the progression of orthotopic N1S1 HCC in rats. This study highlights a concise strategy to prepare pH-responsive and stable LPE-based self-fueling microreactors, which could serve as bifunctional embolic and ferroptosis-inducing agents to enable proof-of-concept transarterial ferro-embolization therapy of HCC.

关键词： CaCO3 nanoparticles Pickering emulsion ferroptosis lipid peroxidation transarterial ferro-embolization

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Synthesis of fluorinated CaCO_(3)-based oxygen-supplying nanophotosensitizers to potentiate photodynamic immunotherapy by reversing tumor hypoxia and immunosuppression

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Nano Research 2023年第7期16卷 9815-9825页

作者： Yunyun Zhang ziliang dong Yu Hao Yimou Gong Chunjie Wang Yifan Yan Minming Chen Yumin Wu Quguang Li Zhuang Liu Liangzhu Feng Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow University199 Ren’ai RoadSuzhou 215123China

Photodynamic therapy is a noninvasive type of phototherapy with a high capacity to boost specific antitumor immunity by causing immunogenic cell death.However,the photodynamic therapeutic potency toward solid tumors is dampened by tumor hypoxia that negatively impairs the generation of cytotoxic singlet oxygen and promotes the formation of tumor immunosuppression.Herein,fluorinated CaCO_(3)(CaF)nanoparticles are prepared with the addition of dopamine-conjugated perfluorosebacic acid and ferric chloride into a calcium chloride ethanol solution via an ammonium bicarbonate-mediated gas-diffusion process.After being coated with commercial lipids and hexadecylamin conjugated chlorin e6(hCe6)via a templated self-assembly process,the yielded PEGylated nanophotosensitizer(hCe6@CaF-PEG)exhibits an effective loading efficiency to perfluoro-15-crown-5-ether(PFCE),a model perfluorocarbon molecule,and thus oxygen molecules.Upon intravenous administration,the obtained PFCE/hCe6@CaF-PEG can alleviate tumor hypoxia by working as an oxygen nanoshuttle.Together with local light emitting diode light exposure,photodynamic treatment with PFCE/hCe6@CaF-PEG can suppress the growth of primary CT26 tumors and unirradiated distant tumors,particularly when synergized with anti-PD-1(aPD-1)immunotherapy to collectively reverse tumor immunosuppression.This work presents an effective strategy to potentiate photodynamic immunotherapy by concurrently reversing tumor hypoxia and immunosuppression.

关键词： photodynamic immunotherapy fluorinated CaCO_(3)nanoparticles oxygen-supplying nanophotosensitizer tumor hypoxia attenuation reversal of tumor immunosuppression

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The acidic tumor microenvironment: a target for smart cancer nano-theranostics

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National Science Review 2018年第2期5卷 269-286页

作者： Liangzhu Feng ziliang dong Danlei Tao Yicheng Zhang Zhuang Liu Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University

The acidic tumor microenvironment(TME), which mainly results from the high glycolytic rate of tumor cells, has been characterized as a hallmark of solid tumors and found to be a pivotal factor participating in tumor progression. Recently, due to the increasing understanding of the acidic TME, it has been shown that the acidic TME could be utilized as a multifaceted target during the design of various pH-responsive nanoscale theranostic platforms for the precise diagnosis and effective treatment of cancers. In this article,we will give a focused overview on the latest progress in utilizing this characteristic acidic TME as the target of nano-theranostics to enable cancer-specific imaging and therapy. The future perspectives in the development of acidic TME-targeting nanomedicine strategies will be discussed afterwards.

关键词： tumor microenvironment cancer targeting nanomedicine theranostics

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NIR-II light activated photodynamic therapy with proteincapped gold nanoclusters

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Nano Research 2018年第10期11卷 5657-5669页

作者： Qian Chen Jiawen Chen Zhijuan Yang Lin Zhang ziliang dong Zhuang Liu Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices Soochow University Suzhou 215123 China Department of Obstetrics and Gynecology The First Affiliated Hospital of Soochow University Suzhou 215123 China

The use of near-infrared （NIR） light for photodynamic therapy （PDT） is a promising strategy to circumvent the limitations of current PDT, in which visible light with limited tissue penetration depth is usually used. In the present stud~ alkyl thiolated gold nanoclusters （AuNCs） were co-modified with human serum albumin （HSA） and catalase （CAT）, and then employed as a multifunctional, optical, theranostic nano-agent. In the AuNC@HSA/CAT system, the AuNCs were able to produce singlet oxygen under excitation by a 1,064-nm laser, which locates in the second NIR window （NIR-II）, and featured much lower tissue absorption and scattering, enabling NIR-II-triggered PDT. The HSA coating greatly improved the physiological stability of the nanoparticles, which showed efficient tumor retention after intravenous injection, as revealed by detecting the AuNC fluorescence. Moreover, the presence of CAT in the nanoparticles triggered decomposition of tumor endogenous H202 to generate oxygen, thereby enhancing the efficacy of PDT by relieving tumor hypoxia. Compared with conventional PDT using visible light, NIR-II-triggered PDT exhibits remarkably increased tissue penetration. Thus, we developed a new type of photosensitizing nano-agent that simultaneously enables in vivo fluorescence imaging, tumor hypoxia relief, and NIR-II light-induced in vivo PDT in the treatment of cancer.

关键词： gold nanoclusters the second near-infrared （NIR-II） light photodynamic therapy tumor hypoxia cancer theranostics

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CaCO3-Assisted Preparation of pH-Responsive Immune-Modulating Nanoparticles for Augmented Chemo-Immunotherapy

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Nano-Micro Letters 2021年第2期13卷 144-161页

作者： Yujie Zhu Zhijuan Yang ziliang dong Yimou Gong Yu Hao Longlong Tian Xianzhu Yang Zhuang Liu Liangzhu Feng Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano and Soft Materials(FUNSOM)Soochow UniversitySuzhou 215123JiangsuPeople’s Republic of China Institutes for Life Sciences School of MedicineSouth China University of TechnologyGuangzhou 510006GuangdongPeople’s Republic of China

Due to the negative roles of tumor microenvironment(TME)in compromising therapeutic responses of various cancer therapies,it is expected that modulation of TME may be able to enhance the therapeutic responses during cancer treatment.Herein,we develop a concise strategy to prepare pH-responsive nanoparticles via the CaCO3-assisted double emulsion method,thereby enabling effective co-encapsulation of both doxorubicin(DOX),an immunogenic cell death(ICD)inducer,and alkylated NLG919(aNLG919),an inhibitor of indoleamine 2,3-dioxygenase 1(IDO1).The obtained DOX/aNLG919-loaded CaCO3 nanoparticles(DNCaNPs)are able to cause effective ICD of cancer cells and at the same time restrict the production of immunosuppressive kynurenine by inhibiting IDO1.Upon intravenous injection,such DNCaNPs show efficient tumor accumulation,improved tumor penetration of therapeutics and neutralization of acidic TME.As a result,those DNCaNPs can elicit effective anti-tumor immune responses featured in increased density of tumor-infiltrating CD8+cytotoxic T cells as well as depletion of immunosuppressive regulatory T cells(Tregs),thus effectively suppressing the growth of subcutaneous CT26 and orthotopic 4T1 tumors on the Balb/c mice through combined chemotherapy&immunotherapy.This study presents a compendious strategy for construction of pH-responsive nanoparticles,endowing significantly enhanced chemo-immunotherapy of cancer by overcoming the immunosuppressive TME.

关键词： CaCO3-assisted double emulsion pH-responsiveness Neutralization of acidic TME Immunosuppressive tumor microenvironment modulation Chemo-immunotherapy

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Metal-polyphenol-network coated CaCO_(3)as pH-responsive nanocarriers to enable effective intratumoral penetration and reversal of multidrug resistance for augmented cancer treatments

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Nano Research 2020年第11期13卷 3057-3067页

作者： ziliang dong Yu Hao Quguang Li Zhijuan Yang Yujie Zhu Zhuang Liu Liangzhu Feng Institute of Functional Nano&Soft Materials Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China

Construction of multifunctional stimuli-responsive nanotherapeutics enabling improved intratumoral penetration of therapeutics and reversal of multiple-drug resistance(MDR)is potent to achieve effective cancer treatment.Herein,we report a general method to synthesize pH-dissociable calcium carbonate(CaCO_(3))hollow nanoparticles with amorphous CaCO_(3)as the template,gallic acid(GA)as the organic ligand,and ferrous ions as the metallic center via a one-pot coordination reaction.The obtained GA–Fe@CaCO_(3)exhibits high loading efficiencies to both oxidized cisplatin prodrug and doxorubicin,yielding drug loaded GA-Fe@CaCO_(3)nanotherapeutics featured in pH-responsive size shrinkage,drug release,and Fenton catalytic activity.Compared to nonresponsive GA-Fe@silica nanoparticles prepared with silica nanoparticles as the template,such GA-Fe@CaCO_(3)confers significantly improved intratumoral penetration capacity.Moreover,both types of drug-loaded GA–Fe@CaCO_(3)nanotherapeutics exhibit synergistic therapeutic efficacies to corresponding MDR cancer cells because of the GA–Fe mediated intracellular oxidative stress amplification that could reduce the efflux of engulfed drugs by impairing the mitochondrial-mediated production of adenosine triphosphate(ATP).As a result,it is found that the doxorubicin loaded GA-Fe@CaCO_(3)exhibits superior therapeutic effect towards doxorubicin-resistant 4T1 breast tumors via combined chemodynamic and chemo-therapies.This work highlights the preparation of pH-dissociable CaCO_(3)-based nanotherapeutics to enable effective tumor penetration for enhanced treatment of drug-resistant tumors.

关键词： self-templated synthesis gallic acid(GA)–Fe@calcium carbonate(CaCO_(3))hollow nanoparticles reactive oxygen species(ROS)generation and chemodynamic therapy improved intratumoral penetration reversal of multi-drug resistance

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Nanoscale covalent organic polymers as a biodegradable nanomedicine for chemotherapy-enhanced photodynamic therapy of cancer

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Nano Research 2018年第6期11卷 3244-3257页

作者： Hairong wang Wenwen Zhu Liangzhu Feng Qian Chen Yu Chao ziliang dong Zhuang Liu Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon Based Functional Materials and DevicesSoochow University Suzhou 215123 China

Recently, covalent-organic polymers （COPs）, which covalently cross-link different types of organic molecules to form organic network structures, have received significant attention in various fields. However, the design of COPs that allows them to act as therapeutic agents remains to be explored. In the present study, a new class of COPs was fabricated by cross-linking the photosensitizer meso-tetra（p-hydroxyphenyl） porphine （THPP） to a chemotherapeutic pro-drug, cis-platinum （IV）; the latter also acts as a reduction-responsive linker. After further conjugation with polyethylene glycol （PEG） in this one-pot reaction, we obtained THPP-Pt-PEG COPs, which can be stored in a lyophilized form and occur as stable nanoparticles in aqueous solution. The THPP-Pt-PEG COPs are effective in killing cancer cells through photodynamic treatment, and exhibited reduction-responsive degradation/drug release behaviors. Upon intravenous injection, the COPs, with a long blood circulation time, showed efficient tumor accumulation. Interestingly, we revealed that after injection of THPP-Pt-PEG COPs, tumors on mice exhibited greatly improved vascular perfusion and largely relieved tumor hypoxia, which favored subsequent photodynamic treatment. Hence, the combined chemo-photodynamic therapy of the COPs offers a remarkably improved therapeutic outcome compared to that with mono-therapies. This work presents a COP-based nanomedicine with high drug loading, lyophilizable formulation, prolonged blood half-life, efficient tumor passive homing, inherent biodegradability, and multiple therapeutic functions to achieve enhanced cancer combination therapy, with promise for clinical translation.

关键词： covalent-organic polymers cisplatin photodynamic therapy drug deliver combination therapy

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Two-dimensional metal-organic-framework as a unique theranostic nano-platform for nuclear imaging and chemo-photodynamic cancer therapy

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Nano Research 2019年第6期12卷 1307-1312页

作者： Wenjun Zhu Yu Yang Qiutong Jin Yu Chao Longlong Tian Jingjing Liu ziliang dong Zhuang Liu Institute of Functional Nano & Soft Materials(FUNSOM) Collaborative Innovation Center of Suzhou Nano Science and TechnologyJiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou 215123China State Key Laboratory of Quality Research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoAvenida da UniversidadTaipaMacao 31608China

Nanoscale metal organic frameworks (NMOFs) with porous structure and inherent biodegradability are attractive nanomedicine platforms.In addition to conventional particulate NMOFs,two-dimensional (2D) NMOFs are emerging as a unique type of NMOFs which however have been relatively less explored for nanomedicine applications.Herein,2D NMOFs composed of Zn2+ and tetrakis(4-carboxyphenyl) porphyrin (TCPP) are fabricated and functionalized with polyethylene glycol (PEG).Compared to their particulate counterpart,such 2D NMOFs show greatly increased drug loading capacity and enhanced light-triggered singlet oxygen production,promising for chemotherapy and photodynamic therapy (PDT),respectively.Utilizing the porphyrin structure of TCPP,our 2D NMOFs could be labeled with a diagnostic radioisotope,99mTc,for single photon emission computer tomography (SPECT) imaging,which reveals efficient tumor homing of those 2D NMOFs upon intravenous injection.While offering a remarkable synergistic in vivo antitumor effect for the combined chemo-PDT,such 2D NMOFs show efficient biodegradation and rapid renal clearance.Our work presents the great promise of 2D NMOFs for nanomedicine applications.

关键词： nanoscale metal-organic-framework two-dimensional nanosheets drug delivery photodynamic therapy combination therapy

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The enhanced permeability and retention effect based nanomedicine at the site of injury

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Nano Research 2020年第2期13卷 564-569页

作者： Yingjun Liu dongdong Sun Qin Fan Qingle Ma ziliang dong Weiwei Tao Huiquan Tao Zhuang Liu Chao Wang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Collaborative Innovation Center of Jiangsu Province of Cancer Prevention and Treatment of Chinese Medicine School of Integrated Chinese and Western MedicineNanjing University of Chinese MedicineNanjing 210023China

The enhanced permeability retention(EPR)effect based nanomedicine has been widely used for tumor targeting during the past decades.Here we unexpectedly observed the similar"EPR effect"at the site of iniury.We found that the temporary dilated and leaky blood vessels caused by the potent vasodilator histamine in response to injury allowed the injected nanoparticles to pass through the vasculature and reached the injured tissue.Our finding shows the potential underline mechanism of"EPR effect"at the injured site.By loading with antibiotics,we further demonstrated a new strategy for prevention of infection at the site of injury.

关键词： enhanced permeability retention(EPR)effect injured tissue polymeric nanoparticles histamine immune response

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超高速激光熔化扫描速度对Al-Mg-Sc高强铝合金性能的影响

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航空材料学报 2024年第1期44卷 133-142页

作者：文聘董子良吴宇董丁炀罗星杜博睿许培鑫陈斐武汉理工大学理学院新材料力学理论与应用湖北省重点实验室武汉430070 中国航发北京航空材料研究院3D打印研究与工程技术中心北京100095 中机新材料研究院郑州有限公司郑州450001 武汉理工大学材料示范学院材料复合新技术国家重点实验室武汉430070

为了明确超高速激光熔化沉积Al-Mg-Sc高强铝合金的沉积态组织及力学性能特征,以7075铝合金为基体,采用自主开发的LDF3000-40型激光熔化沉积设备制备Al-Mg-Sc高强铝合金,探究激光扫描速度对材料微观组织与室温拉伸性能的影响。结果表明:... 详细信息

为了明确超高速激光熔化沉积Al-Mg-Sc高强铝合金的沉积态组织及力学性能特征,以7075铝合金为基体,采用自主开发的LDF3000-40型激光熔化沉积设备制备Al-Mg-Sc高强铝合金,探究激光扫描速度对材料微观组织与室温拉伸性能的影响。结果表明:超高速激光熔化沉积样品均无明显裂纹,但含有少量小尺寸气孔。沉积态组织由细小的α-Al等轴晶及弥散分布的Al_(3)(Sc,Zr)颗粒构成。利用数值模拟进一步研究扫描速度对力学性能的影响,发现在0.1~1 m/s范围内,较高的激光扫描速度能减少粉末材料的堆积,降低沉积层表面的孔隙率,因此可以提高力学性能。沉积态样品最大抗拉强度为303 MPa,断裂伸长率为22.5%。

关键词：超高速激光熔化沉积高强铝合金力学性能数值模拟

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