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Surface Topological Glycosylation-Mediated Mucoadhesion of Bacteria

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Chinese Journal of chemistry 2024年第13期42卷 1447-1455页

作者： Xiao Kuang Xiaobing Liu Ju Chen Wenyan Lv Mengmeng Zhang Huan Chen Feng Wu Jinyao Liu School of Life Sciences Shanghai UniversityShanghai 200444China Shanghai key laboratory for nucleic Acid chemistry and nanomedicine Institute of Molecular MedicineState Key Laboratory of Systems Medicine for CancerRenji HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200127China School of chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and National Center for Translational MedicineShanghai Jiao Tong UniversityShanghai 200240China College of chemistry and Materials Science Shanghai Normal UniversityShanghai 200234China

Sugar moieties present on bacterial surface serve as pivotal regulators of bacterial *** adjusting the abundance and distribution of surface sugar moieties can offer an important approach to manipulating bacterial behavior,but has been proven to be ***,surface topological glycosylation is reported to mediate the interaction of bacteria with mucous *** functionalized by sugar moieties with different branching are synthesized through iterative Michael addition and amide condensation *** a copper-catalyzed azide-alkyne cycloaddition,the resulting compounds with different branching structures can be attached onto bacterial surface that is modified with azido *** a proof-of-concept study,a set of topologically glycosylated probiotics(TGPs)is prepared using linear,two-branched,and tetra-branched compounds,*** interaction between mucin and TGPs was studied and the results demonstrate that,compared to unmodified bacteria,TGPs exhibit an enhanced adhesive capacity to mucin,which increases with the branching *** binding trend is observed in ex vivo colonic mucus adhesion experiments and bacteria glycosylated with tetra-branched compounds display the highest binding *** work proposes a chemical method to tune the abundance and distribution of sugar moieties on bacteria,providing unique significant insights into the manipulation of bacterial behavior through surface modification.

关键词： Topochemistry Bacteria Glycosylation Surface modification Mucoadhesion Click chemistry

Two-color emissive AIEgens with anti-Kasha property for dual-organelle imaging and phototherapy

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Science China chemistry 2024年第5期67卷 1740-1752页

作者： Pu Chen Guogang Shan Qingli Nie Yuting Yan Pengfei Zhang Zujin Zhao Hai-Tao Feng Ben Zhong Tang AIE Research Center Shaanxi Key Laboratory of PhytochemistryCollege of Chemistry and Chemical EngineeringBaoji University of Arts and SciencesBaoji 721013China institute of Functional Material chemistry and National&Local United Engineering Lab for Power Battery Faculty of ChemistryNortheast Normal UniversityChangchun 130024China College of chemistry&Materials Science Northwest UniversityXi’an 710127China Guangdong key laboratory of nanomedicine CAS-HK Joint Lab of BiomaterialsCAS Key Laboratory of Biomedical Imaging Science and SystemShenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China State key laboratory of Luminescent Materials and Devices Key Laboratory of Luminescence from Molecular Aggregates of Guangdong ProvinceSouth China University of TechnologyGuangzhou 510640China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-induced emission luminogens(AIEgens)with donor-π-acceptor structures were designed and synthesized, namely QT-1 and QF-2. Both two AIEgens exhibited excitation wavelength-dependence defying the Kasha's rule, and could stain lipid droplets(LDs) and mitochondria in blue and red fluorescence, respectively. Moreover, thanks to the near-infrared emission and abundant reactive oxygen species(ROS) generation efficiency of QT-1, it was chosen as a photodynamic therapy agent to selectively kill cancer cells from normal cells. Upon light irradiation, an obvious decrease of mitochondrial membrane potential(MMP) and serious change of mitochondrial shape in cells were observed, which corresponded to the efficient inhibition of tumor growth in vivo. This work afforded a promising strategy for the construction of multicolor emission by tuning anti-Kasha behaviors and expanding their application in dualorganelle targeting-based phototheranostics.

关键词： aggregation-induced emission anti-Kasha luminescence fluorescent probe bioimaging photodynamic therapy

Palladium-free chemoselective probe for in vivo fluorescence imaging of carbon monoxide

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Chinese Chemical Letters 2024年第9期35卷 223-226页

作者： Gongcheng Ma Qihang Ding Yuding Zhang Yue Wang Jingjing Xiang Mingle Li Qi Zhao Saipeng Huang Ping Gong Jong Seung Kim Guangdong key laboratory of nanomedicine Shenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS-HK Joint Lab for BiomaterialsResearch Laboratory for Biomedical Optics and Molecular ImagingShenzhen Key Laboratory for Molecular ImagingCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China University of Chinese Academy of Sciences Beijing 100049China Department of chemistry Korea UniversitySeoul 02841South Korea School of Chemical Engineering Northwest UniversityXi’an 710069China Cancer Center Institute of Translational MedicineFaculty of Health SciencesUniversity of MacaoMacao 999078China State key laboratory of Fine Chemicals College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China

Carbon monoxide(CO)is a vital intracellular gas messenger known for its cytoprotective and homeostatic *** plays a pivotal role in a myriad of biological ***,the precise detection of CO is of paramount importance in unraveling the intricacies of pathological mechanisms and advancing the development of disease *** herein introduce NFCOP,a state-of-the-art near-infrared(NIR)turn-on fluorescence(FL)probe that has been meticulously designed for highly sensitive,swift and selective imaging of *** NFCOP response occurred rapidly with CO,within just 10 s,and the calculated detection limit for CO was determined to be 0.32μmol/*** investigations conducted at the cellular level and in vivo demonstrated that NFCOP possesses high sensitivity and selectivity for imaging CO.

关键词： Palladium-free Chemoselective probe Fluorescence imaging Carbon monoxide Near-infrared

D-type neuropeptide decorated AIEgen/RENP hybrid nanoprobes with light-driven ROS generation ability for NIR-Ⅱ fluorescence imaging-guided through-skull photodynamic therapy of gliomas

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Aggregate 2024年第1期5卷 185-195页

作者： Xuelu He Yuan Luo Yanying Li Yuanbo Pan Ryan T.K.Kwok Lulu He Xiaolin Duan Pengfei Zhang Aiguo Wu Ben Zhong Tang 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 SciencesNingboP.R.China Guangdong key laboratory of nanomedicine Shenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS-HK Joint Lab for BiomaterialsResearch Laboratory for Biomedical Optics and Molecular ImagingShenzhen Key Laboratory for Molecular ImagingCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhenP.R.China Department of chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced StudyThe Hong Kong University of Science and Technology(HKUST)KowloonP.R.China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhenP.R.China

Glioma is one of the most common malignant tumors of the central nervous system,leading high mortality rates in ***-induced emission(AIE)photosensitizers-based photodynamic therapy(PDT)has emerged as a promising therapeutic strategy for least-invasive treatment of glioma,which involves local irradiation of the tumor using an external near-infrared(NIR)***,most AIE photosensitizers suffered from poorly penetration of the visible light excitation,bad spatiotemporal resolution in deep tissues and low efficient blood-brain barrier(BBB)crossing ability,which greatly limited the clinical practice of AIE photosensitizers for especially deep-seated brain tumor *** this work,we developed a multifunctional NIR-driven theranostic agent through hybrid of AIE photosensitizers TIND with rare-earth doping nanoparticles(RENPs)NaGdF4:Nd/Yb/Tm with up/down dual-mode conversion *** theranostic agent was further decorated with D-type neuropeptide DNPY for crossing BBB and targeting *** the 808-nm light irradiation,the down-conversion NIR-II luminescence could indicate the position glioma and the upconversion NIR-I luminescence could trigger the AIE photosensitizers producing reactive oxygen species to inhibit orthotopic glioma tumor growth in *** results demonstrate that the integration of Dtype neuropeptide,AIE photosensitizers and RENPs could be promising candidates for in vivo NIR-II fluorescence image-guided through-skull PDT treatments of brain tumors.

关键词： aggregation-induced emission D-type neuropeptide glioma photodynamic therapy rare-earth doping nanoparticles

DMF-scMT-seq linking methylome and transcriptome within single cells with digital microfluidics

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Science China chemistry 2024年第6期67卷 2070-2078页

作者： Xing Xu Xi Zeng Xin Lin Shiyan Lin Shanshan Liang Tian Tian Rui Su Jia Song Chaoyong Yang Collaborative Innovation Center of chemistry for Energy Materials The MOE Key Laboratory of Spectrochemical Analysis and InstrumentationState Key Laboratory of Physical Chemistry of Solid SurfacesDepartment of Chemical BiologyCollege of Chemistry and Chemical EngineeringThe First Affiliated Hospital of Xiamen UniversityXiamen UniversityXiamen361005China institute of molecular Medicine Renji HospitalShanghai Jiao Tong University School of MedicineShanghai200127China chemistry and Materials Science College Shanghai Normal UniversityShanghai200234China chemistry and Biomedicine Innovation Center(ChemBIC) School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China

Single-cell joint analysis of methylome and transcriptome reveals how the methylation regulates the transcriptional ***,traditional bench-top protocols for single-cell DNA methylation and RNA transcription co-detection are laborintensive,cost-ineffective and ***,we establish the DMF-sc MT-seq,a highly-efficient and cost-effective method to simultaneously analyze single-cell DNA methylation and transcriptional activity based on digital *** MT-seq automates the workflow of single-cell isolation,cellular hypotonic lysis,nucleic acid separation and methylome/transcriptome library construction in a contactless and addressable *** system ensures high accuracy(R>0.85),high gene detection ability(14,697 genes per cell at 4 million sequencing depth),and high CpG coverage(677,198 CpG sites per cell at 1million sequencing depth).By using DMF-sc MT-seq,the relationship of DNA methylation and RNA transcription under different genomic contexts is *** further apply DMF-sc MT-seq to study the dynamics of transcription regulation with methylation-inhibiting anti-tumor Decitabine,and identify the methylated promoter/gene body driven genes in response to Decitabine ***-sc MT-seq facilitates the construction of the correlation of DNA methylation and transcriptional activity at the single-cell level in a flexible,sensitive and accurate way,which is anticipated to be a powerful tool in studying single-cell biological systems.

关键词： single-cell analysis digital microfluidics methylome sequencing transcriptome sequencing

NIR-Ⅱ成像引导的精准光动力治疗通过干扰糖代谢重编程增强肿瘤饥饿治疗

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Science Bulletin 2024年第9期69卷 1263-1274页

作者：吴夏维凡勇王楷若缪云秋常永亮明江王欣月陆晟威刘芮池张凡张扬秦环龙施剑林 nanomedicine and Intestinal Microecology Research Center Shanghai Tenth People’s HospitalSchool of MedicineTongji UniversityShanghai 200072China Department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsState Key Laboratory of Molecular Engineering of Polymers and iChemFudan UniversityShanghai 200433China State key laboratory of High Performance Ceramics and Superﬁne Microstructure Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China

Metabolic reprogramming is a mechanism by which cancer cells alter their metabolic patterns to promote cell proliferation and growth, thereby enabling their resistance to external stress. 2-Deoxy-Dglucose(2DG) can eliminate their energy source by inhibiting glucose glycolysis, leading to cancer cell death through starvation. However, a compensatory increase in mitochondrial metabolism inhibits its efficacy. Herein, we propose a synergistic approach that combines photodynamic therapy(PDT) with starvation therapy to address this challenge. To monitor the nanodrugs and determine the optimal triggering time for precise tumor therapy, a multifunctional nano-platform comprising lanthanide-doped nanoparticle(Ln NP) cores was constructed and combined with mesoporous silicon shells loaded with2DG and photosensitizer chlorin e6(Ce6) in the mesopore channels. Under 980 nm near-infrared light excitation, the downshifted 1550 nm fluorescence signal in the second near-infrared(NIR-II, 1000–1700 nm) window from the Ln NPs was used to monitor the accumulation of nanomaterials in ***, upconverted 650 nm light excited the Ce6 to generate singlet oxygen for PDT, which damaged mitochondrial function and enhanced the efficacy of 2DG by inhibiting hexokinase 2 and lactate dehydrogenase A expressions. As a result, glucose metabolism reprogramming was inhibited and the efficiency of starvation therapy was significantly enhanced. Overall, the proposed NIR-II bioimaging-guided PDT-augmented starvation therapy, which simultaneously inhibited glycolysis and mitochondria, facilitated the effects of a cancer theranostic system.

关键词： Metabolic reprogramming Colorectal cancer Glycolytic inhibition Photodynamic therapy NIR-II imaging

Immune checkpoint inhibition mediated with liposomal nanomedicine for cancer therapy

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Military Medical Research 2024年第1期11卷 98-114页

作者： Guang-Long Ma Wei-Feng Lin Faculty of Medicine Centre for Cancer ImmunologyUniversity of SouthamptonSouthampton SO166YDUK Department of molecular chemistry and Materials Science Weizmann Institute of Science76100 RehovotIsrael key laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191China

Immune checkpoint blockade(ICB)therapy for cancer has achieved great success both in clinical results and on the *** the same time,success drives more attention from scientists to improve ***,only a small portion of patients are responsive to this therapy,and it comes with a unique spectrum of side effects termed immunerelated adverse events(irAEs).The use of nanotechnology could improve ICBs’delivery to the tumor,assist them in penetrating deeper into tumor tissues and alleviate their *** nanomedicine has been investigated and used for decades,and is well-recognized as the most successful nano-drug delivery *** successful combination of ICB with liposomal nanomedicine could help improve the efficacy of ICB *** this review,we highlighted recent studies using liposomal nanomedicine(including new emerging exosomes and their inspired nanovesicles)in associating ICB therapy.

关键词： Liposome Exosome Immune checkpoint blockade(ICB)

Supercritical fluid technology:A game-changer for biomacromolecular nanomedicine preparation and biomedical application

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Chinese Chemical Letters 2024年第7期35卷 89-99页

作者： Yating Zheng Yulan Huang Jing Luo Xuqi Peng Xiran Gui Gang Liu Yang Zhang State key laboratory of Vaccines for Infectious Diseases Xiang An Biomedicine LaboratoryNational Innovation Platform for Industry-Education Integration in Vaccine ResearchState Key Laboratory of Molecular Vaccinology and Molecular DiagnosticsCenter for Molecular Imaging and Translational MedicineSchool of Public HealthXiamen UniversityXiamen 361102China Shen Zhen Research institute of Xiamen University Shenzhen 518057China Division of Urology and Department of Surgery Brigham and Women's HospitalHarvard Medical SchoolBostonMA 02115United States Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Biomacromolecules are attractive in biomedical applications as therapeutic agents and potential drug carriers due to their natural active components,good biocompatibility,and high ***,their large relative molecular weight,complex structure,susceptibility to degradation,and poor stability limit their *** can address these issues by improving the therapeutic value,bioavailability,permeability,and absorption of biomacromolecules while regulating their retention time in the ***,compelling evidence has been reported that supercritical fluid(SCF)technology has emerged as an alternative that maintains the integrity of biomacromolecules and reduces environmental *** this review,we highlight a set of unique nanosizing strategies based on SCF technology for biomacromolecular nanomedicine,and extensively discuss their characteristics and *** particular,the protein-based,nucleic acid-based,and polysaccharide-based nanomedicine preparations via SCF technology and their biomedical applications are summarized,and the potential for industrial production of biomacromolecular drugs is also *** further provide perspectives on the opportunities and challenges in this excellent field of biomacromolecular drugs nanotechnology.

关键词： Biomacromolecules Supercritical fluid technology Therapeutic proteins Gene therapy nanomedicine

A multi-parameter-induced activation of gas therapeutic platform to remarkably amplify photodynamic therapy efficacy

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Science China chemistry 2024年第7期67卷 2403-2411页

作者： Jie Sun Ziwen Zhang Hongyu Wu Xuemei Dong Chengjun Dong Lixin Sun Zhiqian Guo Yingchao Liu Xianfeng Gu Chunchang Zhao key laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Department of Medicinal chemistry School of PharmacyFudan UniversityShanghai 201203China Shandong Provincial Hospital Affiliated to Shandong First Medical University Shandong First Medical University&Shandong Academy of Medical ScienceJinan 250021China

Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT *** uncontrolled leakage of gas molecules during delivery seriously hinders its practical biological ***,we report a multifunction nanomedicine that enables precise gas therapy(including carbon monoxide(CO)release and H_(2)S depletion)using a multi-parameter-induced activation gas release strategy,enlarging the PDT *** nanomedicine uses a disulfide bond to covalently link a photosensitizer with the CO donor 3-hydroxyflavone(3-HF).The disulfide bond can be specifically consumed in H_(2)S-rich tumor areas,releasing the CO donor(3-HF),and also depleting H_(2)*** importantly,the photo-controlled production of^(1)O_(2)can induce 3-HF precise release of CO in the tumor *** H_(2)S,light,and^(1)O_(2)multi-parameter-induced activation of gas release strategy ensures the accuracy of GT to amplify PDT *** expected,in vitro and in vivo investigations show that GT makes up for the PDT limitation,exhibiting the highest tumor therapeutic *** multi-parameter-activated design strategy provides a new way to improve the precision and efficacy of multimodal synergistic therapy of tumors.

关键词： gas therapy precision gas release hydrogen sulfide depletion photodynamic therapy multimodal synergistic therapy