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Dual-responsive supramolecular photodynamic nanomedicine with activatable immunomodulation for enhanced antitumor therapy

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Acta Pharmaceutica Sinica B 2024年第2期14卷 765-780页

作者： siqin he Lulu Wang Dongxu Wu Fan Tong Huan Zhao Hanmei Li Tao Gong Huile Gao Yang Zhou Key Laboratory of Tropical Biological Resources of Ministry of Education School of Pharmaceutical SciencesHainan UniversityHaikou 570200China Key Laboratory of Drug-Targeting and Drug Delivery System West China School of PharmacySichuan UniversityChengdu 610041China Revvity Inc. WalthamMA 02451USA School of Food and Biological Engineering Chengdu UniversityChengdu 610106China

A major challenge facing photodynamic therapy(PDT) is that the activity of the immuneinduced infiltrating CD8^(+)T cells is subject to the regulatory T lymphocytes(Tregs), leaving the tumor at risk of recurrence and metastasis after the initial ablation. To augment the antitumor response and reprogram the immunosuppressive tumor microenvironment(TME), a supramolecular photodynamic nanoparticle(DACss) is constructed by the host-guest interaction between demethylcantharidin-conjugated β-cyclodextrin(DMC-CD) and amantadine-terminated disulfide-conjugated FFVLGGGC peptide with chlorin e6 decoration(Ad-ss-pep-Ce6) to achieve intelligent delivery of photosensitizer and immunomodulator for breast cancer treatment. The acid-labile β-carboxamide bond of DMC-CD is hydrolyzed in response to the acidic TME, resulting in the localized release of DMC and subsequent inhibition of Tregs.The guest molecule Ad-ss-pep-Ce6 can be cleaved by a high level of intracellular GSH, reducing photosensitizer toxicity and increasing photosensitizer retention in the tumor. With a significant increase in the CTL/Treg ratio, the combination of Ce6-based PDT and DMC-mediated immunomodulation adequately achieved spatiotemporal regulation and remodeling of the TME, as well as improved primary tumor and in situ lung metastasis suppression with the aid of PD-1 antibody.

关键词： Photodynamic therapy Immunosuppressive microenvironment Immunomodulator Dual-responsive Supramolecularassembly Checkpointblockade

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Kinetic network models to elucidate aggregation dynamics of aggregation-induced emission systems

Aggregate

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Aggregate 2024年第1期5卷 1-8页

作者： Zige Liu Michae L.Kalin Bojun Liu siqin Cao Xuhui Huang Theoretical Chemistry Institute Department of ChemistryUniversity of Wisconsin-MadisonMadisonWisconsinUSA Biophysics University of Wisconsin-MadisonMadisonWisconsinUSA

Aggregation-induced emission(AIE)is a phenomenon where a molecule that is weakly or non-luminescent in a diluted solution becomes highly emissive when aggregated.AIE luminogens(AIEgens)hold promise in diverse applications like bioimaging,chemical sensing,and optoelectronics.Investigation in AIE luminescence is also critical for understanding aggregation kinetics as the aggregation process is an essential component of AIE emission.Experimental investigation of AIEgen aggregation is challenging due to the fast timescale of the aggregation and the amorphous aggregate structures.Computer simulations such as molecular dynamics(MD)simulation provide a valuable approach to complement experiments with atomic-level knowledge to study the fast dynamics of aggregation processes.However,individual simulations still struggle to systematically elucidate heterogeneous kinetics of the formation of amorphous AIEgen aggregates.Kinetic network models(KNMs),constructed from an ensemble of MD simulations,hold great potential in addressing this challenge.In these models,dynamic processes are modeled as a series ofMarkovian transitions occurring among metastable conformational states at discrete time intervals.In this perspective article,we first review previous studies to characterize the AIEgen aggregation kinetics and their limitations.We then introduce KNMs as a promising approach to elucidate the complex kinetics of aggregations to address these limitations.More importantly,we discuss our perspective on linking the output of KNMs to experimental observations of time-resolved AIE luminescence.We expect that this approach can validate the computational predictions and provide great insights into the aggregation kinetics for AIEgen aggregates.These insights will facilitate the rational design of improved AIEgens in their applications in biology and materials sciences.

关键词： hydrophobic aggregation kinetic network models molecular dynamics simulations

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Bias distribution and regulation in photoelectrochemical overall water-splitting cells

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National Science Review 2024年第4期11卷 141-150页

作者： Kun Dang siqin Liu Lei Wu Daojian Tang Jing Xue Jiaming Wang Hongwei Ji Chuncheng Chen Yuchao Zhang Jincai Zhao Key Laboratory of Photochemistry CAS ResearchEducation Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

The water oxidation half-reaction at anodes is always considered the rate-limiting step of overall water splitting（OWS）,but the actual bias distribution between photoanodes and cathodes of photoelectro chemical（PEC） OWS cells has not been investigated systematically.In this work,we find that,for PEC cells consisting of photoanodes（nickel-modified n-Si [Ni/n-Si] and α-Fe2O3） with low photovoltage(Vphhe Pt cathode for satisfying the hydrogen evolution thermodynamics,showing a thermodynamics-controlled characteristic.In contrast,for photoanodes（TiO2and BiVO4） with Vph> 1V,the bias required for cathode activation can be significantly reduced,exhibiting a kinetics-controlled characteristic.Further investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction couplings.Accordingly,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC cells.Motivated by this,an unbiased PEC cell consisting of a simple Ni/n-Si photoanode and Pt cathode is assembled,delivering a photo current density of 5.3±0.2 mA cm-2.

关键词： photoelectrochemistry overall reaction cell bias distribution photoanode water splitting

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Co-delivery of photosensitizer and diclofenac through sequentially responsive bilirubin nanocarriers for combating hypoxic tumors

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Acta Pharmaceutica Sinica B 2022年第3期12卷 1416-1431页

作者： Yang Zhou Fan Tong Weilong Gu siqin he Xiaotong Yang Jiamei Li Yue-Dong Gao Huile Gao 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 PharmacySichuan UniversityChengdu 610064China Core Technology Facility of Kunming Institute of Zoology Chinese Academy of SciencesKunming 650223China Chinese Academy of Sciences Territorial Core Facility of Kunming Biological Diversity Regional Center Kunming 650223China

Considering that photodynamic therapy(PDT)-induced oxygen consumption and microvascular damage could exacerbate hypoxia to drive more glycolysis and angiogenesis, a novel approach to potentiate PDT and overcome the resistances of hypoxia is avidly needed. herein, morpholine-modified PEGylated bilirubin was proposed to co-deliver chlorin e6, a photosensitizer, and diclofenac(Dc). In acidic milieu, the presence of morpholine could enable the nanocarriers to selectively accumulate in tumor cells, while PDT-generated reactive oxidative species(ROS) resulted in the collapse of bilirubin nanoparticles and rapid release of Dc. Combining with Dc showed a higher rate of apoptosis over PDT alone and simultaneously triggered a domino effect, including blocking the activity and expression of lactate dehydrogenase A(LDHA), interfering with lactate secretion, suppressing the activation of various angiogenic factors and thus obviating hypoxia-induced resistance-glycolysis and angiogenesis. In addition, inhibition of hypoxia-inducible factor-1a(HIF-1a) by Dc alleviated hypoxia-induced resistance. This study offered a sequentially responsive platform to achieve sufficient tumor enrichment, on-demand drug release and superior anti-tumor outcomes in vitro and in vivo.

关键词： Bilirubin nanoparticles ROS-responsive drug release Charge reversal Photodynamic therapy Hypoxia Diclofenac LDHA inhibition HIF-1a inhibition

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Blastoids generated purely from embryonic stem cells both in mice and humans

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Science China(Life Sciences) 2024年第2期67卷 418-420页

作者： Baojiang Wu Yanqiu Wang Jia Yan Mengya Liu Xihe Li Fuchou Tang siqin Bao The State Key Laboratory of Reproductive Regulation and Breeding of Grassland Livestock Inner Mongolia UniversityHohhot 010020China Research Center for Animal Genetic Resources of Mongolia Plateau College of Life SciencesInner Mongolia UniversityHohhot 010020China Beijing Advanced Innovation Center for Genomics and Biomedical Pioneering Innovation Center College of Life SciencesPeking UniversityBeijing 100871China Inner Mongolia Saikexing Institute of Breeding and Reproductive Biotechnology in Domestic Animal Hohhot 011517China

Dear Editor,Embryonic stem cells(ESCs)and trophoblast stem cells(TSCs)are derived from blastocysts(Lu et al.,2001).Blastocyst-like structures(blastoids)are self-assembled structures formed by a combination of ESCs and TSCs(Rivron et al.,2018).To increase the success rate of blastoid formation and its similarity with the features of blastocysts,some reports showed that blastoid could also be derived from a combination of three cell lines,ESCs,TSCs,and extraembryonic endoderm cells(XENs),or novel type of stem cells(Sozen et al.,2018;Weatherbee et al.,2023:Wu et al.,2023;Zhang et al.,2023;Zhang et al.,2019).

关键词： purely similarity

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Highly dispersive tetrahedral vanadium species on pure silica ZSM-12 zeolite boosting the selective oxidation of cyclohexane into cyclohexanone

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Science China Chemistry 2024年第7期67卷 2206-2214页

作者： Menglin Xie Ting Li Chao Wu Xiaoling Liu Jinling Ni siqin Yao Yu Zhou Shibo Xi Jun Wang State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Institute of Sustainability for Chemicals Energy and Environment(ISCE2)Agency for ScienceTechnology and Research(A*STAR)Singapore 627833Republic of Singapore College of Materials Science and Engineering Sichuan UniversityChengdu 610065China

The selective oxidation of cyclohexane is a promising green route for the production of KA oil(cyclohexanol and cyclohexanone),but remains a huge challenge to design high-performing heterogeneous catalysts under mild conditions.herein,a pure silica ZSM-12(MTW topology)zeolite was applied as the support to immobilize highly dispersive tetrahedrally coordinated vanadium(V)species and the constructed catalyst 1%V/SZ-12 exhibited high efficiency in the fast and selective oxidation of cyclohexane into cyclohexanone with H2O2.The reaction completed within 30 s,affording the selectivity of 99%towards cyclohexanone and the extremely high turnover frequency(TOF)of 5,891 h^(-1).1%V/SZ-12 was facilely reused with stable activity and feasibly extended to the oxidation of various cyclohexane derivatives.The one-dimensional 12-membered ring microchannels contributed to the formation and accessibility of tetrahedrally coordinated high valent V5+species as the robust active centers,which activated H2O2to generate V–O–O·,the active oxygen species for the electrophilic attack on cyclohexane to produce cyclohexanone as the sole product.

关键词： zeolite metal doping cyclohexane oxidation heterogeneous catalysis

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Hollow copper sulfide nanoparticles carrying ISRIB for the sensitized photothermal therapy of breast cancer and brain metastases through inhibiting stress granule formation and reprogramming tumor-associated macrophages

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Acta Pharmaceutica Sinica B 2023年第8期13卷 3471-3488页

作者： Fan Tong Haili Hu Yanyan Xu Yang Zhou Rou Xie Ting Lei Yufan Du Wenqin Yang siqin he Yuan Huang Tao Gong Huile Gao Key Laboratory of Drug Targeting and Drug Delivery Systems West China School of PharmacySichuan UniversityChengdu 610041China

As known,the benefits of photothermal therapy(PTT)are greatly limited by the heat tolerance of cancer cells resulting from overexpressed heat shock proteins(HSPs).Then HSPs further trigger the formation of stress granules(SGs)that regulate protein expression and cell viability under various stress conditions.Inhibition of SG formation can sensitize tumor cells to PTT.herein,we developed PEGylated pH(low)insertion peptide(PEG-pHLIP)-modified hollow copper sulfide nanoparticles(HCuS NPs)encapsulating the SG inhibitor ISRIB,with the phase-change material lauric acid(LA)as a gatekeeper,to construct a pH-driven and NIR photo-responsive controlled smart drug delivery system(IL@H-PP).The nano medicine could specifically target slightly acidic tumor sites.Upon irradiation,IL@H-PP realized PTT,and the light-controlled release of ISRIB could effectively inhibit the formation of PTT-induced SG to sensitize tumor cells to PTT,thereby increasing the antitumor effect and inducing potent immunogenic cell death(ICD).Moreover,IL@H-PP could promote the production of reactive oxygen species(ROS)by tumor-associated macrophages(TAMs),repolarizing them towards the M1 phenotype and remodeling the immunosuppressive microenvironment.In vitro/vivo results revealed the potential of PTT combined with SG inhibitors,which provides a new paradigm for antitumor and antimetastases.

关键词： Hollow coppersulfide nanoparticles Sensitized PTT SG inhibition TAMs repolarization pH-driven targeting Photothermal responsiveness Immunotherapy Anti-metastases

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Sequential delivery of PD-1/PD-L1 blockade peptide and IDO inhibitor for immunosuppressive microenvironment remodeling via an MMP-2 responsive dual-targeting liposome

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Acta Pharmaceutica Sinica B 2023年第5期13卷 2176-2187页

作者： Chuan Hu Yujun Song Yiwei Zhang siqin he Xueying Liu Xiaotong Yang Tao Gong Yuan Huang Huile Gao Key Laboratory of Drug Targeting and Drug Delivery Systems West China School of PharmacySichuan UniversityChengdu 610041China

Intelligent responsive drug delivery system opens up new avenues for realizing safer and more effective combination immunotherapy.herein,a kind of tumor cascade-targeted responsive liposome(NLG919@Lip-pep1)is developed by conjugating polypeptide inhibitor of PD-1 signal pathway(AUNP-12),which is also a targeted peptide that conjugated with liposome carrier through matrix metalloproteinase-2(MMP-2)cleavable peptide(GPLGVRGD).This targeted liposome is prepared through a mature preparation process,and indoleamine-2,3-dioxygenase(IDO)inhibitor NLG919 was encapsulated into it.Moreover,mediated by the enhanced permeability and retention effect(EPR effect)and AUNP-12,NLG919@Lip-pep1 first targets the cells that highly express PD-L1 in tumor tissues.At the same time,the over-expressed MMP-2 in the tumor site triggers the dissociation of AUNP-12,thus realizing the precise block of PD-1 signal pathway,and restoring the activity of T cells.The exposure of secondary targeting moduleⅡVRGDC-NLG919@Lip mediated tumor cells targeting,and further relieved the immunosuppressive microenvironment.Overall,this study offers a potentially appealing paradigm of a high efficiency,low toxicity,and simple intelligent responsive drug delivery system for targeted drug delivery in breast cancer,which can effectively rescue and activate the body's anti-tumor immune response and furthermore achieve effective treatment of metastatic breast cancer.

关键词： Immunotherapy Cascade targeting Liposome MMP-2 responsive Breast cancer ICBs IDO inhibitors Immunosuppressive microenvironment

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Application Effect of health Management in Community Diabetic Population

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Journal of Biosciences and Medicines 2024年第6期12卷 13-18页

作者： Honglei Wang siqin Ye School of Management Engineering Wanjiang University of Technology Maanshan China IASO Biotherapeutics Nanjing China

Objective: This study aims to improve the health level of patients with diabetes in the community through health management measures under the concept of health management. Methods: Community residents were selected to detect, collate and analyze the social demographic information, body mass index, fasting blood glucose and blood lipid level of diabetic patients before and after health management. Results: The study showed that after the implementation of health management education in the community, the detection rate of diabetes patients increased, but the population was no longer mainly elderly patients, but mainly people under 60 years old. The levels of body mass index, fasting blood glucose, triglyceride (TG), total cholesterol (TC) and low-density lipoprotein (LDL) were significantly decreased (all P Conclusion: Through the investigation of patients before and after health management in residential communities, this study shows that the correct implementation of health management can effectively improve the physiological indicators of diabetes patients, improve the level of health quality, and provide a reference for the prevention and treatment of diabetes patients in communities.

关键词： Community Management Diabetes Mellitus health Education Influencing Factor

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Mechanisms and therapeutic strategies to combat the recurrence and progression of hepatocellular carcinoma after thermal ablation

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Journal of Interventional Medicine 2023年第4期6卷 159-168页

作者： Feilong Ye Lulu Xie Licong Liang Zhimei Zhou siqin he Rui Li Liteng Lin Kangshun Zhu Laboratory of Interventional Radiology Department of Minimally Invasive Interventional Radiology and Department of RadiologyThe Second Affiliated Hospital of Guangzhou Medical University250 East Changgang RoadGuangzhouGuangdong Province510260China

Thermal ablation(TA),including radiofrequency ablation(RFA)and microwave ablation(MWA),has become the main treatment for early-stage hepatocellular carcinoma(HCC)due to advantages such as safety and minimal invasiveness.However,HCC is prone to local recurrence,with more aggressive malignancies after TA closely related to TA-induced changes in epithelial-mesenchymal transition(EMT)and remodeling of the tumor microenvironment(TME).According to many studies,various components of the TME undergo complex changes after TA,such as the recruitment of innate and adaptive immune cells,the release of tumor-associated antigens(TAAs)and various cytokines,the formation of a hypoxic microenvironment,and tumor angiogenesis.Changes in the TME after TA can partly enhance the anti-tumor immune response;however,this response is weak to kill the tumor completely.Certain components of the TME can induce an immunosuppressive microenvironment through complex interactions,leading to tumor recurrence and progression.How the TME is remodeled after TA and the mechanism by which the TME promotes HCC recurrence and progression are unclear.Thus,in this review,we focused on these issues to highlight potentially effective strategies for reducing and preventing the recurrence and progression of HCC after TA.

关键词： hepatocellular carcinoma Thermal ablation Microenvironment Recurrence and progression Therapeutic strategies

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