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Tumor inflammation-specific self-amplifying fluorescent molecular probes induce an anti-tumor immune response

Science China Chemistry 2025年第1期 273-287页

作者： Shuguang Yang Lijun Hu Hong xiao zecong xiao Xintao Shuai PCFM Lab of Ministry of Education School of Materials Science and Engineering Sun Yat-sen University Department of Ultrasound The Fifth Affiliated Hospital Sun Yat-sen University Department of Medical Ultrasound The Third Affiliated Hospital of Sun Yat-sen University Nanomedicine Research Center The Third Affiliated Hospital of Sun Yat-sen University

Enhancing the concentration of exogenous molecular drugs within the tumor microenvironment through enzyme-catalyzed polymerization presents a novel strategy for cancer therapy. Nonetheless, the optimization of the catalytic efficiency is often impeded by the inefficient expression of enzymes. Herein, we reported a self-amplifying fluorescent molecular probe, Bis-HTPICG, for photodynamic therapy(PDT) and subsequent PDT-induced immunoreaction. The Bis-HTP-ICG probe possesses a noticeable enzyme-catalyzed polymerization facilitated by myeloperoxidase(MPO), a crucial enzyme secreted by neutrophils at inflammation sites. Upon exposure to laser irradiation, Bis-HTP-ICG showed a high PDT efficacy, inducing an acute inflammatory response that stimulates further recruitment of neutrophils and then elevated MPO secretion. The heightened level of MPO enhances the accumulation of the Bis-HTP-ICG via self-polymerization or binding with intratumoral proteins following MPO enzyme catalysis, instigating a self-amplifying chain reaction cycle involving Bis-HTP-ICG, neutrophils and ***, PDT efficiently incites immunogenic cell death(ICD) in tumor cells, initiating an anti-tumor immune response including dendritic cells(DCs) maturation, T cell proliferation and reprogramming of tumor-associated neutrophils(TANs). This work portrays a promising strategy for self-amplification of fluorescent molecular probes through adjustable enzyme levels,potentially offering a unique avenue to enhance the tumor accumulation of molecular drugs for improved tumor therapy.

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Harnessing the potential of hydrogels for advanced therapeutic applications: current achievements and future directions

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Signal Transduction and Targeted Therapy 2024年第8期9卷 3176-3241页

作者： Pelin Lu Dongxue Ruan Meiqi Huang Mi Tian Kangshun Zhu Ziqi Gan zecong xiao Nanomedicine Research Center The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhou 510630PR China Department of Minimally Invasive Interventional Radiology and Laboratory of Interventional RadiologyThe Second Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510260PR China State Key Laboratory of Respiratory Disease National Clinical Research Center for Respiratory DiseaseNational Center for Respiratory MedicineDepartment of Respiratory and Critical Care MedicineGuangzhou Institute for Respiratory HealthThe First Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510120PR China Department of Stomatology Chengdu Second People's HospitalChengdu 610021PR China Hospital of Stomatology Guangdong Provincial Key Laboratory of StomatologyGuanghua School of StomatologySun Yat-sen UniversityGuangzhou 510055PR China

The applications of hydrogels have expanded significantly due to their versatile,highly tunable properties and breakthroughs in biomaterial *** this review,we cover the major achievements and the potential of hydrogels in therapeutic applications,focusing primarily on two areas:emerging cell-based therapies and promising non-cell therapeutic *** the context of cell therapy,we discuss the capacity of hydrogels to overcome the existing translational challenges faced by mainstream cell therapy paradigms,provide a detailed discussion on the advantages and principal design considerations of hydrogels for boosting the efficacy of cell therapy,as well as list specific examples of their applications in different disease *** then explore the potential of hydrogels in drug delivery,physical intervention therapies,and other non-cell therapeutic areas(e.g.,bioadhesives,artificial tissues,and biosensors),emphasizing their utility beyond mere delivery ***,we complement our discussion on the latest progress and challenges in the clinical application of hydrogels and outline future research directions,particularly in terms of integration with advanced biomanufacturing *** review aims to present a comprehensive view and critical insights into the design and selection of hydrogels for both cell therapy and noncell therapies,tailored to meet the therapeutic requirements of diverse diseases and situations.

关键词： directions overcome breakthrough

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Nanodrug enhances post-ablation immunotherapy of hepatocellular carcinoma via promoting dendritic cell maturation and antigen presentation

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Bioactive Materials 2023年第3期21卷 57-68页

作者： zecong xiao Tan Li Xinyao Zheng Liteng Lin xiaobin Wang Bo Li Jingjun Huang Yong Wang Xintao Shuai Kangshun Zhu Department of Minimally Invasive Interventional Radiology And Laboratory of Interventional RadiologyThe Second Affiliated Hospital of Guangzhou Medical UniversityGuangzhou510260China Nanomedicine Research Center The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhou510630China College of Chemistry and Materials Science Jinan UniversityGuangzhou510632China Department of Dermatology The Nanfang Hospital of Southern Medical UniversityGuangzhouGuangdong510515China

Thermal ablation(TA)as an effective method treating hepatocellular carcinoma(HCC)in clinics is facing great challenges of high recurrence and *** immune-checkpoint blockade(ICB)-based immuno-therapy has shown potential to inhibit recurrence and metastasis,the combination strategy of ICB and thermal ablation has shown little progress in HCC *** tremendous hurdle for combining ICB with thermal ablation lies with the insufficient antigen internalization and immaturity of tumor-infiltrating dendritic cells(TIDCs)which leads to an inferior immune response to distant tumor growth and ***,an antigen-capturing nanoplatform,whose surface was modified with mannose as a targeting ligand,was constructed for co-delivering tumor-associated antigens(TAAs)and m6A demethylases inhibitor(i.e.,fat mass and obesity asso-ciated gene(FTO)inhibitor)into *** vivo results demonstrate that the intratumoral injection of nanodrug followed by HCC thermal ablation promotes dendritic cells(DCs)maturation,improves tumor infiltration of effector T cells and generates immune memory,which synergize with ICB treatment to inhibit the distant tumor growth and lung ***,the antigen-capturing and FTO-inhibiting nanodrug holds potential to boost the ICB-based immunotherapy against HCC after thermal ablation.

关键词： Thermal ablation Tumor-infiltrating dendritic cells N6-methyladenosine modification Nanoplatform Tumor immunotherapy

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Twins-like nanodrugs synchronously transport in blood and coalesce inside tumors for sensitive ultrasound imaging and triggerable penetrative drug delivery

Aggregate

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Aggregate 2024年第3期5卷 175-187页

作者： Yujun Cai Gengjia Chen Minzhao Lin Bo Li Huihai Zhong Tan Li zecong xiao Yong Wang Xintao Shuai PCFM Lab of Ministry of Education School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhouChina Nanomedicine Research Center the Third Afﬁliated Hospital of Sun Yat-sen UniversityGuangzhouChina Department of Radiology The Sixth Afﬁliated HospitalSun Yat-sen UniversityGuangzhouChina College of Chemistry and Materials Science Jinan UniversityGuangzhouChina

Nanodrugs capable of aggregating in the tumor microenvironment(TME)have demonstrated great efﬁciency in improving the therapeutic *** vari-ous approaches,the strategy utilizing electrostatic interaction as a driving force to achieve intratumor aggregation of nanodrugs has attracted great ***,the great difference between the two nanodrugs with varied physicochemical prop-erties makes their synchronous transport in blood circulation and equal-opportunity tumor uptake impossible,which signiﬁcantly detracts from the beneﬁcial effects of nanodrug aggregation inside *** herein propose a new strategy to construct a pair of extremely similar nanodrugs,referred to as“twins-like nanodrugs(TLNs)”,which have identical physicochemical properties including the same morphology,size,and electroneutrality to render them the same blood circulation time and tumor *** 1:1 mixture of TLNs(TLNs-Mix)intravenously injected into a mouse model efﬁciently accumulates in tumor sites and then transfers to oppositely charged nanodrugs for electrostatic interaction-driven coalescence via responding to matrix metalloproteinase-2(MMP-2)enriched in *** addition to enhanced tumor retention,the thus-formed micron-sized aggregates show high echo intensity essen-tial for ultrasound imaging as well as ultrasound-triggered penetrative drug *** to their distinctive features,the TLNs-Mix carrying sonosensitizer,immune adjuvant,and ultrasound contrast agent exert potent sonodynamic immunotherapy against hypovascular hepatoma,demonstrating their great potential in treating solid malignancies.

关键词： intratumor aggregation by coulombic interactions penetrative drug delivery sonodynamic immunother-apy twins-like nanodrugs ultrasound imaging

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Stiffness-tuned and ROS-sensitive hydrogel incorporating complement C5a receptor antagonist modulates antibacterial activity of macrophages for periodontitis treatment

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Bioactive Materials 2023年第7期25卷 347-359页

作者： Ziqi Gan zecong xiao Zhen Zhang Yang Li Chao Liu Xin Chen Yuanbo Liu Dongle Wu Chufeng Liu Xintao Shuai Yang Cao Hospital of Stomatology Guangdong Provincial Key Laboratory of StomatologyGuanghua School of StomatologySun Yat-sen UniversityGuangzhou510055China Nanomedicine Research Center The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhou510630China Stomatological Hospital Southern Medical UniversityGuangzhou510260China

Periodontitis is admittedly a microbe-driven intractable infectious disease,in which Porphyromonas gingivalis(Pg)plays a keystone *** can selectively impair the antimicrobial responses of periodontal resident macrophages including their phagocytic and bactericidal activity without interfering their proinflammatory activity,which leads to microflora disturbance,destructive periodontal inflammation and alveolar bone loss ***,an injectable ROS-sensitive hydrogel is developed for releasing active bone marrow-derived macrophages(named ex-situ macrophages hereafter)and a complement C5a receptor antagonist(C5A)to the gingival *** appropriately tuning the hydrogel stiffness,the phagocytic activity of these macrophages is greatly enhanced,reaching an optimal performance at the elastic modulus of 106 ***,C5A avoids undesired C5a receptor activation by Pg to ensure the bacterial killing activity of both the ex-situ and in-situ ***,the ROS-sensitive hydrogels show another distinct feature of decreasing the ROS level in periodontal niche,which contributes to the alleviated periodontal inflammation and attenuated bone loss as *** study highlights the potential of utilizing hydrogels with tailored biomechanical properties to remodel the functions of therapeutic cells,which is expected to find wide applications even beyond periodontitis treatment.

关键词： Periodontitis treatment Cell therapy ROS-Responsive hydrogels C5a receptor blockade Mechanostimulation

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Thermally activated delayed fluorescence enhanced by macrocyclization

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Science China Chemistry 2025年

作者： Shuo Li Chenghao Zhu Lijun Mao Xin Zhang zecong Ye Chunju Li Da Ma School of Pharmaceutical and Chemical Engineering & Institute for Advanced Studies Taizhou University School of Chemical Engineering and Light Industry Guangdong University of Technology Tianjin Key Laboratory of Structure and Performance for Functional Molecules Tianjin Normal University

Thermally activated delayed fluorescence (TADF) depends on reverse intersystem crossing (RISC) from the lowest triplet to the singlet excited state. Here, a macrocyclization strategy is developed to achieve TADF emission by promoting RISC. 5-(9Hcarbazol-9-yl) isophthalonitrile, a fluorescent molecule, is coupled with 1,4-dimethoxybenzene by methylene bridges to form a macrocycle with TADF emission. Experimental results and theoretical calculation indicate that the macrocyclization strategy contributes to RISC promotion and suppression of nonradiative decay, resulting in effective TADF emission transformed from prompt fluorescence. Three TADF luminophores are cyclized with the same strategy, and an enhanced TADF emission of up to3.8 folds is observed. The marriage of macrocycle chemistry and luminescent materials will provide new guidelines for designing efficient TADF materials.

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Comparison of different valent iron on anaerobic sludge digestion:Focusing on oxidation reduction potential,dissolved organic nitrogen and microbial community

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Frontiers of Environmental Science & Engineering 2022年第6期16卷 159-170页

作者： zecong Yu Keke xiao Yuwei Zhu Mei Sun Sha Liang Jingping Hu Huijie Hou Bingchuan Liu Jiakuan Yang School of Environmental Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China Hubei Provincial Engineering Laboratory of Solid Waste Treatment Disposal and RecyclingWuhan 430074China State Key Laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China

This study compared effects of three different valent iron(Fe^(0),Fe(II)and Fe(III))on enhanced anaerobic sludge digestion,focusing on the changes of oxidation reduction potential(ORP),dissolved organic nitrogen(DON),and microbial *** the same iron dose in range of 0−160 mg/L after an incubation period of 30 days(d),the maximum methane production rate of sludge samples dosed with respective Fe^(0),Fe(II)and Fe(III)at the same concentration showed indiscernible differences at each iron dose,regardless of the different iron ***,their behavior in changes of ORP,DON and microbial community was different:(1)the addition of Fe^(0) made the ORP of sludge more negative,and the addition of Fe(II)and Fe(III)made the ORP of sludge less ***,whether being more or less negative,the changes of ORP may show unobservable effects on methane yield when it ranged from−278.71 to−379.80 mV;(2)the degradation of dissolved organic nitrogen,particularly proteins,was less efficient in sludge samples dosed with Fe^(0) compared with those dosed with Fe(II)and Fe(III)after an incubation period of 30 *** the same dose of 160 mg/L iron,more cysteine was noted in sludge samples dosed with Fe(II)(30.74 mg/L)and Fe(III)(27.92 mg/L)compared with that dosed with Fe^(0)(21.75 mg/L);(3)Fe^(0) particularly promoted the enrichment of Geobacter,and it was 6 times higher than those in sludge samples dosed with Fe(II)and Fe(III)at the same dose of 160 mg/L iron.

关键词： Enhanced anaerobic sludge digestion Different iron valence Oxidation reduction potential Dissolved organic nitrogen Microbial community

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Phase transformation of Cr(Ⅵ)-adsorbed ferr ihydr ite in the presence of Mn(Ⅱ): Fate of Mn(Ⅱ)and Cr(Ⅵ)

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Journal of Environmental Sciences 2022年第3期34卷 251-259页

作者： zecong Ding Guangzhao Sun Fenglian Fu Chujia Ye School of Environmental Science and Engineering Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlGuangdong University of TechnologyGuangzhou 510006China

Ferrihydrite is an important sink for the toxic heavy metal ions, such as Cr(Ⅵ). As ferrihydrite is thermodynamically unstable and gradually transforms into hematite and goethite, the stability of Cr(Ⅵ)-adsorbed ferrihydrite is environmentally significant. This study investigated the phase transformation of Cr(Ⅵ)-adsorbed ferrihydrite at different pH in the presence of aqueous Mn(Ⅱ), as well as the fate of Mn(Ⅱ) and Cr(Ⅵ) in the transformation process of ferrihydrite. Among the ferrihydrite transformation products, hematite was dominant, and goethite was minor. The pre-adsorbed Cr(Ⅵ) inhibited the conversion of ferrihydrite to goethite at initial pH 3.0, whereas little amount of adsorbed Mn(Ⅱ) favored the formation of goethite at initial pH 7.0. After the aging process, Cr species in solid phase existed primarily as Cr(Ⅲ) in the presence of Mn(Ⅱ) at initial pH 7.0 and 11.0. The aqueous Mn concentration was predominantly unchanged at initial pH 3.0, whereas the aqueous Mn(Ⅱ) was adsorbed onto ferrihydrite or form Mn(OH)_(2) precipitates at initial pH 7.0 and 11.0, promoting the immobilization of Cr(Ⅵ). Moreover, the oxidation of Mn(Ⅱ) occurred at initial pH 7.0 and 11.0, forming Mn(Ⅲ/Ⅳ)(hydr)oxides.

关键词： Ferrihydrite Phase transformation Gr(Ⅵ)adsorption and reduction Mn(Ⅱ)adsorption and oxidation

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Anaerobic digestion of sludge by different pretreatments:Changes of amino acids and microbial community

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Frontiers of Environmental Science & Engineering 2022年第2期16卷 109-123页

作者： Keke xiao zecong Yu Kangyue Pei Mei Sun Yuwei Zhu Sha Liang Huijie Hou Bingchuan Liu Jingping Hu Jiakuan Yang School of Environmental Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China Hubei Provincial Engineering Laboratory of Solid Waste Treatment Disposal and Recycle TechnologyWuhan 430074China State Key Laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China

Many studies have investigated the effects of different pretreatments on the performance of anaerobic digestion of ***,the detailed changes of dissolved organic nitrogen,particularly the release behavior of proteins and the byproducts of protein hydrolysis-amino acids,are rarely known during anaerobic digestion of sludge by different *** we quantified the changes of three types of proteins and 17 types of amino acids in sludge samples solubilized by ultrasonic,thermal,and acid/alkaline pretreatments and their transformation during anaerobic digestion of *** protein,aromatic protein I,aromatic protein II,and cysteine were identified as the key dissolved organic nitrogen responsible for methane production during anaerobic digestion of sludge,regardless of the different pretreatment *** from the depletion of other amino acids,cysteine was resistant to degradation after an incubation period of 30 days in all sludge ***,the“cysteine and methionine metabolism(K00270)”was absent in all sludge samples by identifying 6755 Kyoto Encyclopedia of Genes and Genomes assignments of genes *** contributed to the generation of methane and the degradation of acetic,propionic,and n-butyric acids through decreasing oxidation-reduction potential and enhancing biomass *** study provided an alternative strategy to enhance anaerobic digestion of sludge through in situ production of cysteine.

关键词： Sludge pretreatments Dissolved organic nitrogen Proteins Amino acids Structural equation model Metagenomic sequencing analysis

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Manipulating noncovalent conformational lock via side-chain engineering for luminescence at aggregate level

Aggregate

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Aggregate 2024年第4期5卷 349-359页

作者： Mingbing Lian Yingxiao Mu zecong Ye Ziying Lu Jingping xiao Jianyu Zhang Shaomin Ji Haoke Zhang Yanping Huo Ben Zhong Tang School of Chemical Engineering and Light Industry Analytical and Testing CenterGuangdong University of TechnologyGuangzhouChina Stratingh Institute for Chemistry and Zernike Institute for Advanced Materials University of GroningenGroningenThe Netherlands MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhouChina School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongGuangdongChina

The unfavorable photochemical processes at the molecular level have become a bar-rier limiting the use of aromatic amides as high-performance luminescent ***,we propose a reliable strategy for manipulating noncovalent conformational lock(NCL)via side-chain engineering to burst out eye-catching luminescence at the aggregate *** to the invisible emission in dilute solutions,dyad OO with a three-centered H-bond gave the wondrous crystallization-induced emis-sion with a quantum yield of 66.8%and clusterization-triggered emission,which were much brighter than those of *** calculations demonstrate that crystallization-induced planarized intramolecular charge transfer(PICT),con-formation rigidiﬁcation,and through-space conjugation(TSC)are responsible for aggregate-state *** NCL composed of intramolecular N-H⋅⋅⋅Ointeractions could boost molecular rigidity and planarity,thus greatly facilitating PICT and *** study would inspire researchers to design efﬁcient luminescent materials at the aggregate level via rational conformational control.

关键词： aromatic amide clusterization-triggered emission crystallization-induced emission noncovalent confor-mational lock side-chain engineering

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