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Nano Research 2024年第6期17卷 5399-5408页

作者： Xuxuan Gu Jinlong Shen Zhiwei Xu Wenqi Wang Ying Wu Wen Zhou Chen Xie quli fan State Key Laboratory of Organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Nanjing University of Posts&Telecommunications9 Wenyuan RoadNanjing 210023China

Semiconducting polymer nanoparticles(SPNs)have shown great promise in second near-infrared window(NIR-II)phototheranostics.However,the issue of long metabolic time significantly restricts the clinical application of SPNs.In this study,we rationally designed a biodegradable SPN(BSPN50)for NIR-II fluorescence imaging-guided photodynamic therapy(PDT).BSPN50 is prepared by encapsulating a biodegradable SP(BSP50)with an amphiphilic copolymer F-127.BSP50 is composed of NIR-II fluorescent diketopyrrolopyrrole(DPP)segment and degradable poly(phenylenevinylene)(PPV)segment with the ratio of 50/50.BSPN50 has both satisfactory degradability under myeloperoxidase(MPO)/hydrogen peroxide(H_(2)O_(2))and NIR-II fluorescence emission upon 808 nm laser excitation.Furthermore,BSPN50 shows good photodynamic efficacy under 808 nm laser irradiation.BSPN50 shows a faster degradation rate than BSPN100 which has no PPV segment both in vitro and in vivo.In addition,BSPN50 can effectively diagnose tumor via NIR-II fluorescence imaging and inhibit the tumor growth by PDT.Thus,our study provides a rational approach to construct biodegradable nanoplatforms for efficient tumor NIR-II phototheranostics.

关键词： near-infrared(NIR)-II fluorescence imaging semiconducting polymer nanoparticles photodynamic therapy tumor imaging

Advanced technologies for single-cell in situ protein profiling

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Science China Chemistry 2022年第1期65卷 48-67页

作者： Wen Zhou Xiaoyue Ni Chen Xie quli fan Dingbin Liu State Key Laboratory of Organic Electronics and Information Displays and Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Institute of Advanced Materials(IAM)Nanjing University of Posts&TelecommunicationsNanjing 210023China State Key Laboratory of Medicinal Chemical Biology Research Center for Analytical SciencesTianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China

Cells are inherently heterogeneous to achieve a diverse spectrum of biological functions.To understand the underlying protein machinery that achieves these fascinating functions,it is important to develop advanced analytical methods that can profile proteins in their native environment,as protein expression,aggregation,degradation,and regulation define both normal physiology as well as pathogenicity.Genome and transcriptome sequencing have seen major advances at the single-cell levels,but comprehensive proteomic profiling is still challenging.The conventional proteomic methods,such as enzyme-linked immunosorbent assay(ELISA),western blot,and protein chips,can characterize biomarkers of interest.Still,these ensemble techniques are unsuitable for single-cell studies.Increasing evidence has shown the significance of in situ,sensitive,quantitative,and multiplexed profiling of biomarkers in single cells for diagnosis and treatment guidance.Here,we review the recent development of advanced imaging and spectroscopy techniques,including mass cytometry,immunofluorescence,and surfaceenhanced Raman spectrometry(SERS)for single-cell proteomic imaging.We also provide our view on the challenges and the outlook.

关键词： proteomics single-cell CyTOF immunofluorescence SERS

Intelligent polymeric hydrogen sulfide delivery systems for therapeutic applications

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Bioactive Materials 2023年第1期19卷 198-216页

作者： fan Rong Tengjiao Wang Qian Zhou Haowei Peng Jingtian Yang quli fan Peng Li Frontiers Science Center for Flexible Electronics(FSCFE) Xi’an Institute of Flexible Electronics(IFE)&Xi’an Institute of Biomedical Materials and Engineering(IBME)Northwestern Polytechnical University(NPU)127 West Youyi RoadXi’anShaanxi710072PR China National Key Laboratory for Organic Electronics and Information Displays and Institute of Advanced Materials(IAM) Nanjing University of Posts and TelecommunicationsNanjing210023PR China Honors College Northwestern Polytechnical University(NPU)127 West Youyi RoadXi’anShaanxi710072PR China Queen Mary University of London Engineering School Northwestern Polytechnical University(NPU)127 West Youyi RoadXi’anShaanxi710072PR China

Hydrogen sulfide(H_(2)S)plays an important role in regulating various pathological processes such as protecting mammalian cell from harmful injuries,promoting tissue regeneration,and regulating the process of various diseases caused by physiological disorders.Studies have revealed that the physiological effects of H_(2)S are highly associated with its concentrations.At relatively low concentration,H_(2)S shows beneficial functions.However,long-time and high-dose donation of H_(2)S would inhibit regular biological process,resulting in cell dysfunction and apoptosis.To regulate the dosage of H_(2)S delivery for precision medicine,H_(2)S delivery systems with intelligent characteristics were developed and a variety of biocompatibility polymers have been utilized to establish intelligent polymeric H_(2)S delivery systems,with the abilities to specifically target the lesions,smartly respond to pathological microenvironments,as well as real-timely monitor H_(2)S delivery and lesion conditions by incorporating imaging-capable moieties.In this review,we focus on the design,preparation,and therapeutic applications of intelligent polymeric H_(2)S delivery systems in cardiovascular therapy,inflammatory therapy,tissue regenerative therapy,cancer therapy and bacteria-associated therapy.Strategies for precise H_(2)S therapies especially imaging-guided H_(2)S theranostics are highlighted.Since H_(2)S donors with stimuli-responsive characters are vital components for establishing intelligent H_(2)S delivery systems,the development of H_(2)S donors is also briefly introduced.

关键词： Hydrogen sulfide prodrug Smart drug delivery Gas therapy Reactive sulfur species Precision medicine

Highly selective detection of copper(Ⅱ) by a “ligand-free” conjugated copolymer in nucleophilic solvents

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Frontiers of Chemical Science and Engineering 2020年第1期14卷 105-111页

作者： Weixing Deng Pengfei Sun quli fan Lei Zhang Tsuyoshi Minami Key Laboratory for Organic Electronics and Information Displays&Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing University of Posts&TelecommunicationsNanjing 210023China Institute of Industrial Science The University of TokyoMeguro-kuTokyo 153-8505Japan

The synthesis of N-cyclohexyl carbamate-attached fluorene-alt-phenylene copolymer(PFPNCC)and the use of PFPNCC as a“ligand-free”fluorescent chemosensor for Cu(Ⅱ)are described.Addition of Cu(Ⅱ)can efficiently quench the fluorescence of PFPNCC in nucleophilic solvents such as DMF and DMSO,but not in low nucleophilic solvents such as 1,4-dioxane and THF.Ultraviolet-visible spectra of the mixture of the conjugated polymer and Cu(Ⅱ)indicate the presence of a reduced Cu(Ⅰ)ion in the solution.Furthermore,fluorescence recovery of PFPNCC observed at low temperature suggests that the quenching and reducing mechanism is most probably due to a photo-induced electron transfer from excited PFPNCC to Cu(Ⅱ).Our findings provide a novel strategy for highly selective conjugated polymer-based chemosensors for various target analytes,albeit“ligand-free”.

关键词： ligand-free fluorescent chemosensor copper photo-induced electron transfer

Elucidating the excited-state dynamics behavior in near-infrared Bodipy dye and aggregates toward biophotonics

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Science China Chemistry 2020年第8期63卷 1075-1081页

作者： Xiaofei Miao Haojie Tao Wenbo Hu Yonghui Pan quli fan Wei Huang Key Laboratory for Organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Nanjing University of Posts&TelecommunicationsNanjing 210023China Shaanxi Institute of Flexible Electronics(SIFE) Northwestern Polytechnical University(NPU)Xi’an 710072China

Photo-induced excited-state dynamics within organic materials fundamentally determine their photophysical properties for various applications,and thus understanding the primary excited-state dynamics behavior is of fundamental and practical significance.Until recently,the excited-state dynamics of organic materials towards biophotonics have been rarely studied,although numerous endeavors have been devoted to the design of organic materials for biophotonics.Herein,various spectroscopy technologies including femtosecond transient absorption(fs-TA)spectroscopy clearly reveal a totally different excited state dynamics behavior within Bodipy monomer(2B-BDP dye)and aggregates(2B-BDP NPs),indicating strongly morphology dependent character.2B-BDP dye undergoes an ultrafast conversion from S1 to intramolecular charge transfer(ICT)state for subsequent photoluminescence(PL)and nonradiative(NR)decay,while 2B-BDP NPs show an accelerated excited-state deactivation mainly through S1→S0 NR decay.The potential bioapplications based on the corresponding excited state dynamics behavior are discussed together with experimental results.Interestingly,the accelerated NR decay in 2B-BDP NPs does not yield a stronger photoacoustic(PA)signal than that in 2B-BDP dye,which violates the conventional wisdom that faster NR decay would benefit the photothermal effects for better photoacoustic imaging(PAI).These insightful and fundamental observations of the excited-state dynamics may contribute an alternative approach at the molecular level towards the future design of functional Bodipy-based organic molecules with desirable performances.

关键词： excited-state dynamics bodipy organic nanoparticles intramolecular charge transfer photoacoustic imaging

NIR-Ⅱ-absorbing conjugated polymer-based theranostic agent for NIR-Ⅱfluorescence imaging-guided photothermal therapy acting synergistically with tumor microenvironment-responsive nitric oxide therapy

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ChemPhysMater 2022年第1期1卷 51-55页

作者： Jie Li Lisi Xie Wei Sang Wenxi Li Guohao Wang Hao Tian Zhan Zhang Jianhua Liu quli fan Yunlu Dai Cancer Centre and Institute of Translational Medicine Faculty of Health SciencesUniversity of MacaoMacao SAR 999078China Department of Radiology The Second Hospital of Jilin UniversityChangchun 130041China Key Laboratory for Organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing University of Posts&TelecommunicationsNanjing 210023China MoE Frontiers Science Center for Precision Oncology University of MacaoMacao SAR 999078China

Despite tremendous advances in gas therapy,there are major concerns about the inevitable concentration of toxicity and the ability to perform real-time tracking of drug delivery.Second near-infrared(NIR-Ⅱ)window absorbing nanoplatforms hold great promise for precision medicine because of their excellent tissue penetration of light and non-invasive nature.In this study,we engineered an NIR-Ⅱlaser-activated theranostic agent(named CP-bF@PEG)that was composed of amphiphilic polymers(Pluronic F127,with polyethylene glycol,PEG,moieties)coated with an NIR-Ⅱ-absorbing conjugated polymer(PTTBBT,CP)and nitric oxide(NO)donor(benzofuroxan,bF),which served as an NIR-Ⅱphotothermal inducer and NO nanogenerator.Under deep tissue penetration of NIR-Ⅱlaser irradiation,CP-bF@PEG was found to possess fluorescence imaging ability to accurately identify tumor and excellent photothermal effect.Moreover,CP-bF@PEG could generate NO via glutathione activation in the tumor microenvironment in a controllable manner.This NIR-Ⅱ-absorbing polymer for high-contrast NIR-Ⅱfluorescence imaging-guided precision photothermal therapy achieved synergistic effects with NO therapy,as evidenced by pronounced tumor therapeutic efficacy and few side effects.This nanotheranostic agent is a highly promising candidate for high-contrast NIR-Ⅱimaging-guided precision photothermal therapy combined with gas therapy against cancer.

关键词： Conjugated polymer NIR-II fluorescence Photothermal therapy Tumor environment response Nitric oxide therapy

NIR-Ⅱprobe modified by poly(L-lysine)with efficient ovalbumin delivery for dendritic cell tracking

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Science China Chemistry 2020年第9期63卷 1272-1280页

作者： Chao Wang Bo Sun Hui Bao Tao Wang Wenjuan Xu Pengfei Sun quli fan Wei Huang Key Laboratory for Organic Electronics and Information Displays&Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing University of Posts&TelecommunicationsNanjing 210023China Frontiers Science Center for Flexible Electronics&Shaanxi Institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an 710072China

Dendritic cell(DC)vaccine is an effective strategy for cancer immunotherapy by carrying antigen into DCs and migrating these DCs to drain lymph nodes after inoculation.In this article,second near-infrared window(NIR-II)fluorescent nanoparticles have been used to uptake antigen and activate DCs.Ovalbumin(OVA),an antigen for immunization,can be loaded on the surface of these NIR-II fluorescent nanoparticles via electrostatic interaction by virtue of their functionalized poly(L-lysine)(PLL),which exhibits biocompatibility and strong selective interaction with OVA.In addition,these antigen-loaded complexes can efficiently be engulfed by immature DCs to induce DC maturation and cytokine secretion.After subcutaneous injection,highly sensitive NIR-II fluorescence signal from nanoparticles indicates that nanoparticle-labeled DCs can successfully migrate into lymph nodes in vivo,showing great promise in immunotherapy against cancer.

关键词： poly(L-lysine) DC vaccine NIR-Ⅱfluorescence tracking

Near-Infrared-Excitable Organic Ultralong Phosphorescence through Multiphoton Absorption

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Research 2020年第1期2020卷 474-485页

作者： Ye Tao Lele Tang Qi Wei Jibiao Jin Wenbo Hu Runfeng Chen Qingqing Yang Huanhuan Li Ping Li Guichuan Xing quli fan Chao Zheng Wei Huang Key Laboratory for Organic Electronics and Information Displays&Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts&Telecommunications9 Wenyuan RoadNanjing 210023China Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacao 999078China Frontiers Science Center for Flexible Electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KLoFE)Shaanxi Key Laboratory of Flexible ElectronicsXi’an Key Laboratory of Flexible ElectronicsXi’an Key Laboratory of Biomedical Materials&EngineeringXi’an Institute of Flexible ElectronicsInstitute of Flexible Electronics(IFE)Northwestern Polytechnical UniversityXi’an710072 ShaanxiChina

Organic ultralong room-temperature phosphorescence(OURTP)with a long-lived triplet excited state up to several seconds has triggered widespread research interests,but most OURTP materials are excited by only ultraviolet(UV)or blue light owing to their unique stabilized triplet-and solid-state emission feature.Here,we demonstrate that near-infrared-(NIR-)excitable OURTP molecules can be rationally designed by implanting intra/intermolecular charge transfer(CT)characteristics into Haggregation to stimulate the efficient nonlinear multiphoton absorption(MPA).The resultant upconverted MPA-OURTP show ultralong lifetimes over 0.42 s and a phosphorescence quantum yield of~37%under both UV and NIR light irradiation.Empowered by the extraordinary MPA-OURTP,novel applications including two-photon bioimaging,visual laser power detection and excitation,and lifetime multiplexing encryption devices were successfully realized.These discoveries illustrate not only a delicate design map for the construction of NIR-excitable OURTP materials but also insightful guidance for exploring OURTP-based nonlinear optoelectronic properties and applications.

关键词： excited photon Infrared

A Water-soluble Conjugated Polymer for Thiol Detection Based on ＂Tu rn-off＂ Effect

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Chinese Journal of Chemistry 2015年第8期33卷 881-887页

作者： Gaoshan Zeng Jie Li Hao Liang Yan Yuan Xiang Li Chao Yin Zhen Yang quli fan Xiaomei Lu Wei Huang Key Laboratory for Organic Electronics & Information Displays and lnstitute of Advanced Materials Nanjing University of Posts & Telecommunications Nanjing Jiangsu 210046 China Jiangsu-Singapore Joint Research Center for Organic/Bio-Electronics & Information Displays and Institute of Advanced Material Nanjing Tech University Nanjing Jiangsu 211816 China

We investigated a novel water-soluble conjugated polymer （WSCP） for thiol detection based on ＂turn-off＂ ef- fect. This WSCP was modified with poly（ethylene glycol）（PEG） by disulfide linkages to achieve good solubility in aqueous solution （34 mg/mL） and high quantum yield （0.47）. The separation of water-soluble PEG chains from the conjugated backbone induced by the cleavage of the disulfide linkages would lead to a significant decrease of the water solubility and a dramatical fluorescence quenching of the probe. The combined intuitive images and fluores- cence spectrophotometer further confirmed that decreased solubility produced an aggregation of the hydrophobic conjugated backbone. The fluorescence intensity of the probe showed a good linear relationship with glutathione （GSH）（1-200 nmol·L^-1）, and the detection limit was 16 nmol·L^-1. This WSCP probe was confirmed to be a good sensing material with high selectivity to thiols by testing various biological molecules. And this WSCP probe ex- hibited good detection effect to intracellular thiols by testing Hela cells. Considering the good sensitivity and selec- tivity, the probe could be further used in vivo. In conclusion, this conjugated polymer probe made up for the draw- backs of the micromolecue probes and contributed to the development of new probes based on conjugated poly- mers.

关键词： thiols disulfide water-soluble conjugated polymer poly（ethylene glycol）

An Improved Turn-On Aptasensor for Thrombin Detection Using Split Aptamer Fragments and Graphene Oxide

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Chinese Journal of Chemistry 2015年第8期33卷 981-986页

作者： Xingfen Liu Yonghong Yang Xiaoxiao Hua Xiaomiao Feng Shao Su Yanqin Huang quli fan Lianhui Wang Wei Huang Key Laboratory for Organic Electronics & Information Displays and Institute of Advanced Materials NationalJiangsu Synergetie Innovation Center for Advanced Materials Nanjing University of Posts & Telecommunications Nanjing Jiangsu 210023 China Key Laboratory of Flexible Electronics & Institute of Advanced Materials National Jiangsu Synergetic Innovation Center for Advanced Materials Nanjing Teeh University Nanj ing Jiangsu 211816 China

An improved tum-on aptasensor for thrombin detection using split aptamer fragments and graphene oxide （GO） was reported. The thrombin-binding aptamer （Aptl5） was split into two parts for target recognition, an 8-base se- quence labeled with fluorescein （FAM-Apt-A） and a 7-base oligonucleotide sequence （Apt-B）. In the absence of target protein, the fluorescence of FAM-Apt-A/Apt-B was quenched by GO through n-n stacking between GO and single-stranded DNA. However, when thrombin was introduced into the system, a target-induced G-quadruplex forms with two split aptamer fragments and thrombin. The fluorescence recovered due to weak interaction between G-quadruplex and GO. Compared to the strategy using intact aptamer, probe concentration was lowered, and an improved sensitivity was obtained. Moreover, heating process to avoid unfavorable secondary structure was avoided due to the use of shorter split aptamer fragments.

关键词： sensor split aptamer graphene oxide