A novel molecularly imprinted polymer (MIP) based on upconversion nanoparticles (UCNPs) was successfully synthesized for determination of Ochratoxin A (OTA). The MIP was developed on the silica-coated UCNPs using N-(1...A novel molecularly imprinted polymer (MIP) based on upconversion nanoparticles (UCNPs) was successfully synthesized for determination of Ochratoxin A (OTA). The MIP was developed on the silica-coated UCNPs using N-(1-hydroxy-2-naphthoyl amido)-(L)-phenylalanine (HNA-Phe) as the alternative template. The final composite combined the advantages of the high selectivity of MIP with the high fluorescence intensity of UCNPs which was selective and sensitive to OTA. Under the optimal condition, the fluorescence intensity of UCNPs@SiO2@MIP decreases linearly when the concentration of OTA increases from 0.05 to 1.0 mg/L. The detection limit of OTA with the method was 0.031 mg/L. At three spiked concentration levels (50, 100 and 200 μg/kg), the recovery ranges of OTA in corn, rice and feed are 88.0%–91.6%, 80.2%–91.6% and 89.2%–90.4%, respectively.展开更多
Fluorescently encoded microbeads are in demand for multiplexed applications in different fields.Compared to organic dye-based commercially available Luminex's x MAP technology, upconversion nanoparticles(UCNPs) ar...Fluorescently encoded microbeads are in demand for multiplexed applications in different fields.Compared to organic dye-based commercially available Luminex's x MAP technology, upconversion nanoparticles(UCNPs) are better alternatives due to their large antiStokes shift, photostability, nil background, and single wavelength excitation. Here, we developed a new multiplexed detection system using UCNPs for encoding poly(ethylene glycol) diacrylate(PEGDA) microbeads as well as for labeling reporter antibody. However, to prepare UCNPs-encoded microbeads, currently used swellingbased encapsulation leads to non-uniformity, which is undesirable for fluorescence-based multiplexing. Hence,we utilized droplet microfluidics to obtain encoded microbeads of uniform size, shape, and UCNPs distribution inside. Additionally, PEGDA microbeads lack functionality for probe antibodies conjugation on their surface.Methods to functionalize the surface of PEGDA microbeads(acrylic acid incorporation, polydopamine coating)reported thus far quench the fluorescence of UCNPs. Here,PEGDA microbeads surface was coated with silica followed by carboxyl modification without compromising the fluorescence intensity of UCNPs. In this study, droplet microfluidics-assisted UCNPs-encoded microbeads of uniform shape, size, and fluorescence were prepared.Multiple color codes were generated by mixing UCNPs emitting red and green colors at different ratios prior to encapsulation. UCNPs emitting blue color were used to label the reporter antibody. Probe antibodies were covalently immobilized on red UCNPs-encoded microbeads for specific capture of human serum albumin(HSA) as a model protein. The system was also demonstrated for multiplexed detection of both human C-reactive protein(hCRP) and HSA protein by immobilizing anti-h CRP antibodies on green UCNPs.展开更多
We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To impro...We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To improve the energy transfer efficiency,UCNPs and CdS nanoparticles were bound in close proximity to each other within the SiO2matrix.β‐NaYF4:Yb(30%),Tm(0.5%)@NaYF4:Yb(20%),Er(2%)core–shell nanoparticles were used as nanotransducers for near infrared light.These nanoparticles exhibited enhanced upconversion fluorescence compared withβ‐NaYF4:Yb(30%),Tm(0.5%)orβ–NaYF4:Yb(30%),Tm(0.5%)@NaYF4nanoparticles.The morphologies,size and chemical compositions have been extensively investigated using field emission scanning electron microscopy(FESEM),transmission electron microscopy(TEM),X‐ray diffraction(XRD)and X‐ray photoelectron spectra(XPS),respectively.The TEM images showed that the TiO2composite nanotubes were embedded with a large amount of UCNPs and CdS nanoparticles.The composite TiO2nanotubes degraded more than90%of rhodamine B(RhB)dye during20min of irradiation by simulated solar light.In particular,more than50%of RhB was decomposed in70min,under irradiation of near infrared light(NIR).This high degradation was attributed to the full spectrum absorption of solar light,and the enhanced transfer efficiency for near infrared light.The as‐prepared nanostructures can harness solar energy,and provide an alternative to overcome energy shortages and environmental protection.展开更多
Two-photon luminescence with near-infrared(NIR)excitation of upconversion nanoparticles(NPs)is of great importance in biological imaging due to deep penetration in high-scattering tissues,low auto-luminescence and goo...Two-photon luminescence with near-infrared(NIR)excitation of upconversion nanoparticles(NPs)is of great importance in biological imaging due to deep penetration in high-scattering tissues,low auto-luminescence and good sectioning ability.Unfortunately,common two-photon luminescence is in visible band with an extremely high exciation power density,which limits its application.Here,we synthesized NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs with strong twophoton NIR emission and a low excitation power density.Furthermore,NaYF_(4):Yb/Tm@NaYF_(4)@SiO_(2)@OTMS@F127 NPs with high chemical stability were obtained by a modified multilayer coating method which was applied to upconversion NPs for thefirst time.In addition,it is shown that the as-prepared hydrophillic upconversion NPs have great biocompatibility and kept stable for 6 hours during in vivo whole-body imaging.The vessels with two-photon luminescence were clear even under an excitation power density as low as 25mW/cm^(2).Vivid visualizations of capillaries and vessels in a mouse brain were also obtained with low background and high contrast.Because of cheaper instruments and safer power density,the NIR two-photon luminescence of NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs could promote wider application of two-photon technology.The modified multilayer coating method could be widely used for upconversion NPs to increase the stable time of the in vivo circulation.Our work possesses a great potential for deep imaging and imaging-guided treatment in the future.展开更多
To better utilize the infrared(IR)region in sunlight for photovoltaic devices(PVs),upconversion nanoparticles(UCNPs)have been proposed to improve power conversion efficiency(PCE).However,researchers recently have foun...To better utilize the infrared(IR)region in sunlight for photovoltaic devices(PVs),upconversion nanoparticles(UCNPs)have been proposed to improve power conversion efficiency(PCE).However,researchers recently have found that the upconversion(UC)effect is negligible in PVs performance improvement for their ultra-low UC photoluminescence quantum yields of UCNPs solid film,while the real mechanism of UCNPs in PVs has not been clearly studied.Herein,based on the material inorganic perovskitesγ-CsPbI_(3),NaYF_(4):20%Yb^(3+),2%Er^(3+)UCNPs were integrated into different transport layer to optimize device performance.Compared with reference device,the short-circuit current density and PCE of optimized device reached 20.87 mA/cm^(2)(20.39 mA/cm^(2))and 18.34%(17.72%),respectively,without sacrificing open-circuit voltage and filling factor.Further experimental characterizations verified that the improved performance was attributable to enhanced visible light absorption instead of IR.To theoretically explain the statement,the light field distribution in device was simulated and the absorption in different layers was calculated.The results revealed that the introduction of UCNPs with different refractive index from other layers caused light field disturbance,and improved visible light captured by γ-CsPbI_(3).Importantly,through experiments and theoretical calculation,the research deeply explored the potential mechanism of UCNPs in optimizing PVs performance.展开更多
Luminescent properties of Er^(3+)-and Yb^(3+)-co-doped CaF_(2)upconversion nanoparticles(UCNPs)were investigated in single particle and densely-packed states with a custom-built microscope.The single UCNPs exhibit lin...Luminescent properties of Er^(3+)-and Yb^(3+)-co-doped CaF_(2)upconversion nanoparticles(UCNPs)were investigated in single particle and densely-packed states with a custom-built microscope.The single UCNPs exhibit linear dependency of luminescent intensity on excitation power while the densely-packed UCNPs exhibit a 2-order power law-dependency indicating a two-photon absorption process.Time-domain luminescence intensity measurements were performed and the curves were fitted to excitationnemission rate functions based on a simplified three-state model.The results indicate that the intermediates in single particles are much less and saturated in a short time,and there are strong couplings of the ground states and intermediate states between neighboring UCNPs in densely packed UCNPs.展开更多
Highly toxic reactive oxygen species(ROS)induced apoptosis and ferroptosis have been considered as significant cell death pathways for cancer therapy.However,insufficient amount of intracellular ROS extremely restrict...Highly toxic reactive oxygen species(ROS)induced apoptosis and ferroptosis have been considered as significant cell death pathways for cancer therapy.However,insufficient amount of intracellular ROS extremely restricts the therapeutic effect.Toward this,we report a rationally designed nanocomposite(mUCC)with enhanced ROS generation ability,inducing the combination of apoptosis and ferroptosis through synergistic photodynamic therapy(PDT)and chemodynamic therapy(CDT).Under 808 nm near-infrared(NIR)light irradiation,photocatalytic reaction is triggered starting from the separation of electron-hole pairs on the surface of heterojunction(CeO_(2)/CuO),realizing improved ROS production.Simultaneously,mUCC served as Fenton-like agent exhibits considerable ability to generate highly toxic·OH under tumor microenvironment(TME).The boosted accumulation of ROS disrupts the redox balance within tumor cells and results in the integration of apoptosis and ferroptosis.In addition,mUCC shows satisfactory tumor targeting property benefiting from the cancer cell membrane functionalization under the guidance of magnetic resonance imaging(MRI)and NIR fluorescence imaging.The intelligent mUCC with good biocompatibility and excellent antitumor response achieves efficient tumor elimination under synergistic PDT and CDT.This work offers an elective approach for further development of ROS-based therapeutic nanoplatform in cancer therapy.展开更多
Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications s...Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing,photocatalysis,anticounterfeiting and nanomedicine.However,precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth mechanisms.Herein,we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites(ZIF-8=zeolitic imidazolate framework-8).The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission,which were verified by steady-state/transient photoluminescence(PL)spectroscopy and single-particle imaging.Ethylenediamine(EDA)was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the composites.By adjusting the concentration of EDA from 0 to 25 mmol/L,the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron(RD)to truncated rhombic dodecahedron(TRD),cube with truncated edges(CTE),cube,and finally a unique form of interpenetration twins(IT).The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy(SEM)images and the formation mechanism was thoroughly revealed.Furthermore,we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and shapes.The proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications.展开更多
As a widespread element,heavy metals have a significant impact on human health and threaten human health.It is of great significance to develop analytical technologies that can detect heavy metal ions quickly and accu...As a widespread element,heavy metals have a significant impact on human health and threaten human health.It is of great significance to develop analytical technologies that can detect heavy metal ions quickly and accurately.In comparison to conventional fluorescent materials such as organic dyes,quantum dot(QD)labels,and carbon quantum dots(CD),fluorescence detection technology utilizing lanthanide(Ln)ion-doped upconversion nanoparticles(UCNPs)stands out due to its distinctive attributes.These include a notably reduced autofluorescence background,enhanced tissue penetration capabilities,biocompatibility with cellular tissues,and minimal photodamage inflicted on biological samples.The utilization of this technology has garnered considerable attention across multiple fields.In the domain of heavy metal detection,traditional laboratory methods necessitate costly instrumentation and a fully equipped laboratory,involving intricate sample processing procedures and protracted detection periods,as well as a demand for skilled personnel.In contrast,the implementation of this material offers rapid and cost-effective detection,significantly mitigating the technical barriers for operators.Consequently,this represents an exceptional avenue to curtail expenses and broaden the scope of detection within the analytical process.This paper reviews the research progress of UCNPs in the detection of heavy metal ions,encompassing a brief elucidation of the luminescence principle of upconversion nanomaterials and commonly used detection principles.Additionally,it provides a detailed overview of the research status of several common non-metal ions and essential heavy metals.Furthermore,it summarizes the current focal points in UCNP detection and discusses the challenges and prospects associated with it.展开更多
Lanthanide-based upconversion nanoparticles(UCNPs)have been widely explored in various fields,including optical imaging,in recent years.Although earlier work has shown that UCNPs with different lanthanide(Ln3+)dopants...Lanthanide-based upconversion nanoparticles(UCNPs)have been widely explored in various fields,including optical imaging,in recent years.Although earlier work has shown that UCNPs with different lanthanide(Ln3+)dopants exhibit various colors,multicolor-especially in vivo multiplexed biomedical imaging-using UCNPs has rarely been reported.In this work,we synthesize a series of UCNPs with different emission colors and functionalize them with an amphiphilic polymer to confer water solubility.Multicolor in vivo upconversion luminescence(UCL)imaging is demonstrated by imaging subcutaneously injected UCNPs and applied in multiplexed in vivo lymph node mapping.We also use UCNPs for multicolor cancer cell labeling and realize in vivo cell tracking by UCL imaging.Moreover,for the first time we compare the in vivo imaging sensitivity of quantum dot(QD)-based fluorescence imaging and UCNP-based UCL imaging side by side,and find the in vivo detection limit of UCNPs to be at least one order of magnitude lower than that of QDs in our current non-optimized imaging system.Our data suggest that,by virtue of their unique optical properties,UCNPs have great potential for use in highly-sensitive multiplexed biomedical imaging.展开更多
Upconversion nanoparticles(UCNPs)doped with lanthanides can convert near-infrared excitation into UV and visible emissions.Because of their relatively high emission efficiency,UCNPs are appealing materials for use in ...Upconversion nanoparticles(UCNPs)doped with lanthanides can convert near-infrared excitation into UV and visible emissions.Because of their relatively high emission efficiency,UCNPs are appealing materials for use in a variety of sectors.UCNPs are known for low auto-fluorescence,excellent chemical and thermal photo-stability,deep tissue penetration,exceptional biocompatibility,low toxicity,color purity,and ease of surface functionalization.In this review,we explain a few recent strategies to boost the efficiency and luminescence of upconversion nanoparticles and minimize quenching by fabricating them as core/shell,nanofibers,or heavily doped lanthanides.Applications of UCNPs in drug delivery,Photodynamic therapy(PDT),biosensors,bioimaging,and optogenetics are also discussed along with their mechanism of action.Our motivation for this review is to understand the working mechanism of UCNPs and their applications in various fields.展开更多
UCNPs@AgBiS_(2) core-shell nanoparticles that AgBiS_(2) coated on the surface of upconversion nanoparticles (UCNPs) was successfully prepared through an ion exchange reaction. The photothermal conversion efficiency of...UCNPs@AgBiS_(2) core-shell nanoparticles that AgBiS_(2) coated on the surface of upconversion nanoparticles (UCNPs) was successfully prepared through an ion exchange reaction. The photothermal conversion efficiency of AgBiS_(2) can be improved from 14.7% to 45% due to the cross relaxation between Nd ions and AgBiS_(2). The doping concentration of Nd ions played a critical role in the production of reactive oxygen species (ROS) and enhanced the photothermal conversion efficiency. The NaYF4:Yb/Er/Nd@NaYF4:Nd nanoparticles endows strong upcon-version emissions when the doped concentration of Nd ions is 1% in the inner core, which excites the AgBiS_(2) shell to produce ROS for photodynamic therapy (PDT) of cancer cells. As a result, the as-prepared NaYF4:Yb/Er/ Nd@NaYF4:Nd@AgBiS_(2) core-shell nanoparticles showed combined photothermal/photodynamic therapy (PTT/ PDT) against malignant tumors. This work provides an alternative near-infrared light-active multimodal nano-structures for applications such as fighting against cancers.展开更多
Counterfeit leather products infringe the intellectual property rights of the business,cause enormous economic loss,and negatively influence the business enthusiasm for innovation.However,traditional anti-counterfeiti...Counterfeit leather products infringe the intellectual property rights of the business,cause enormous economic loss,and negatively influence the business enthusiasm for innovation.However,traditional anti-counterfeiting materials for leather products suffer from complicated fabrication procedures,photobleaching,and high volatile organic com-pound(VOC)emissions.Here,a sustainable and invisible anti-counterfeiting ink composed of waterborne polyure-thane and water-dispersible lanthanide-doped upconversion nanoparticles(UCNPs)featuring ease of preparation,high photostability,non-toxicity,low VOC emissions,and strong adhesion strength for leather products is designed and synthesized.After decorating on the surface of leather products,the obtained patterns are invisible under normal light conditions.Upon irradiation at 808 nm,the invisible patterns can be observed by naked eyes due to the visible light emitted by 808 nm excited UCNPs.Our approach described here opens a new pathway to realize the long-term,stable anti-counterfeiting function of leather products.展开更多
Thromboembolism is the leading cause of cardiovascular mortality.Currently,for the lack of targeting,short half-life,low bioavailability and high bleeding risk of the classical thrombolytic drugs,pharmacological throm...Thromboembolism is the leading cause of cardiovascular mortality.Currently,for the lack of targeting,short half-life,low bioavailability and high bleeding risk of the classical thrombolytic drugs,pharmacological thrombolysis is usually a slow process based on micro-pumping.In addition,frequently monitoring and regulating coagulation functions are also required during(and after)the process of thrombolysis.To address these issues,a targeted thrombolytic and anticoagulation nanoplatform(UCATS-UK)is developed based on upconversion nanoparticles(UCNPs)that can convert 808 or 980 nm near-infrared(NIR)light into UV/blue light.This nanoplatform can target and enrich in the thrombus site.Synergistic thrombolysis and anticoagulation therapy thus could be realized through the controlled release of urokinase(UK)and nitric oxide(NO).Both in vitro and in vivo experiments have confirmed the excellent thrombolytic and anticoagulative capabilities of this multifunctional nanoplatform.Combined with the unique fluorescent imaging capability of UCNPs,this work is expected to contribute to the development of clinical thrombolysis therapy towards an integrated system of imaging,diagnosis and treatment.展开更多
Real-time exploring the cellular endocytic pathway of viral capsid proteins(VCPs)functionalized nanocargos at the single-particle level can provide deep insight into the kinetic information involved in virus infection...Real-time exploring the cellular endocytic pathway of viral capsid proteins(VCPs)functionalized nanocargos at the single-particle level can provide deep insight into the kinetic information involved in virus infection.In this work,porcine circovirus type 2(PCV2)VCPs with different functions are modified onto the surface of upconversion nanoparticles(VCPs-UCNPs)to investigate the cellular internalization process in real-time.Clathrin-mediated endocytosis is found to be the essential uptake mechanism for these VCPs-UCNPs.Besides,it is verified that P_(1)-UCNPs(PCV2 VCPs with nuclear localization signal,namely P1)can be easily assembled close to the perinuclear area,which is different from that of P_(2)-UCNPs(PCV2 VCPs without nuclear localization signal,namely P_(2)).Interestingly,multistep entry processes are observed.Particularly,confined diffusion is observed during the transmembrane process.The intracellular transport of VCPs-UCNPs is dependent on microtubules toward the cell interior.During this process,P_(1)-UCNPs display increased velocities with active transport,while diffusion much faster around the perinuclear area.But for P_(2)-UCNPs,there are only two phases involved in their endocytosis process.This study presents distinct dynamic mechanisms for the nanocargos with different functions,which would make a useful contribution to the development of robust drug delivery systems.展开更多
We demonstrate the fabrication of a new DNA sensor that is based on the optical interactions occurring between oligonucleotide-coated NaYF4:Yb^(3+);Er^(3+) upconversion nanoparticles and the two-dimensional dichalcoge...We demonstrate the fabrication of a new DNA sensor that is based on the optical interactions occurring between oligonucleotide-coated NaYF4:Yb^(3+);Er^(3+) upconversion nanoparticles and the two-dimensional dichalcogenide materials,MoS_(2) and WS_(2).Monodisperse upconversion nanoparticles were functionalized with single-stranded DNA endowing the nanoparticles with the ability to interact with the surface of the two-dimensional materials via van der Waals interactions leading to subsequent quenching of the upconversion fluorescence.By contrast,in the presence of a complementary oligonucleotide target and the formation of double-stranded DNA,the upconversion nanoparticles could not interact with MoS_(2) and WS_(2),thus retaining their inherent fluorescence properties.Utilizing this sensor we were able to detect target oligonucleotides with high sensitivity and specificity whilst reaching a concentration detection limit as low as 5 mol·L^(-1),within minutes.展开更多
Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 n...Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 nm irradiation. The application of 808 nm laser as the excitation source could achieve better penetration depth and avoid overheating problem. The combination of UCNPs and RBS could realize the on-demand release of NO at desired time and location by simply controlling the output of NIR laser.Cellular uptake results showed that more nanoparticles were internalized in cancer stem-like cells(CSCs)rather than non-CSCs. Therefore, a synergistic cancer therapy strategy to eradicate both CSCs and nonCSCs simultaneously was developed. Traditional chemo-drug could inhibit non-CSCs but has low killing efficiency in CSCs. However, we found that the combination of NO and chemotherapy could efficiently inhibit CSCs in bulk cells, including inhibiting mammosphere formation ability, decreasing CD44^+/CD24^- subpopulation and reducing tumorigenic ability. The mechanism studies confirmed that NO could not only induce apoptosis but also increase drug sensitivity by declining drug efflux in CSCs. This UCNPsbased platform may provide a new combinatorial strategy of NO and chemotherapy to improve cancer treatment.展开更多
Although small EVs(sEVs)have been used widely as biomarkers in disease diagnosis,their heterogeneity at single EV level has rarely been revealed.This is because high-resolution characterization of sEV presents a major...Although small EVs(sEVs)have been used widely as biomarkers in disease diagnosis,their heterogeneity at single EV level has rarely been revealed.This is because high-resolution characterization of sEV presents a major challenge,as their sizes are below the optical diffraction limit.Here,we report that upconversion nanoparticles(UCNPs)can be used for super-resolution profiling the molecular heterogeneity of sEVs.We show that Er3+-doped UCNPs has better brightness and Tm3+-doped UCNPs resulting in better resolution beyond diffraction limit.Through an orthogonal experimental design,the specific targeting of UCNPs to the tumour epitope on single EV has been cross validated,resulting in the Pearson’s R-value of 0.83 for large EVs and~65%co-localization double-positive spots for sEVs.Furthermore,super-resolution nanoscopy can distinguish adjacent UCNPs on single sEV with a resolution of as high as 41.9 nm.When decreasing the size of UCNPs from 40 to 27 nm and 18 nm,we observed that the maximum UCNPs number on single sEV increased from 3 to 9 and 21,respectively.This work suggests the great potentials of UCNPs approach“digitally”quantify the surface antigens on single EVs,therefore providing a solution to monitor the EV heterogeneity changes along with the tumour progression progress.展开更多
Multimodal imaging nanoprobes are urgently sought because they can integrate different imaging func- tion into individual nanoplatform and provide more comprehensive and accurate information for the diagnosis of early...Multimodal imaging nanoprobes are urgently sought because they can integrate different imaging func- tion into individual nanoplatform and provide more comprehensive and accurate information for the diagnosis of early-stage tumor. Lanthanide-based upconversion nanoparticles (UCNPs) are regarded as promising nanoplatforms to fabricate these probes. Herein, we firstly developed the active core-active shell structured NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs with the average diameter of 13.23 + 0.96 nm as multimodal imaging probes. These water-dispersible nanoprobes presented excellent near-infrared to near-infrared (NIR-to-NIR) upconversion luminescence (UCL) performance, which is favorable for optical bioimaging due to deeper tissue penetration and autofluorescence reduction. After coated with the NaGdF4:Yb active shell, the UCL emission intensity at 800 nm increased by 7.2 times. These nanoprobes exhibited a desirable longitudinal relaxivity (rl = 3.58 L/(mmol s)) and strong X-ray attenuation property (58.84 HU L/g). The cytotoxicity assessment, histology analysis and biodistribution study revealed that NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs had relatively low cytotoxicity and negligible organ toxicity. These UCNPs were applied for NIR-to-NIR UCL imaging in vivo. More importantly, the detection of small tumor was successfully achieved under Trweighted MRI and CT imaging modalities after intravenous injection of these UCNPs. These results revealed that NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs could serve as promising NIR-to-NIR UCL/MRI/CT trimodal imaging probes.展开更多
One dimensional(1D)nanostructures attract considerable attention,enabling a broad application owing to their unique properties.However,the precise mechanism of 1D morphology attainment remains a matter of debate.In th...One dimensional(1D)nanostructures attract considerable attention,enabling a broad application owing to their unique properties.However,the precise mechanism of 1D morphology attainment remains a matter of debate.In this study,ultrafast picosecond(ps)laser-induced treatment on upconversion nanoparticles(UCNPs)is offered as a tool for 1 D-nanostructures formation.Fragmentation,reshaping through recrystallization process and bioadaptation of initially hydrophobic(β-Na_(1.5)Y_(1.5_)F_(6):Yb^(3+),Tm^(3+)/β-Na_(1.5)Y_(1.5_)F_(6))core/shell nanoparticles by means of one-step laser treatment in water are demonstrated.“True”1D nanostructures through"Medusa^-like structures can be obtained,maintaining anti-Stokes luminescence functionalities.A matter of the one-dimensional UCNPs based on direction of energy migration processes is debated.The proposed laser treatment approach is suitable for fast UCNP surface modification and nano-to-nano transformation,that open unique opportunities to expand UCNP applications in industry and biomedicine.展开更多
基金Project(17ZYPTJC00050)supported by Science and Technology Committee of Tianjin,ChinaProject(2017YFC1600803)supported by the Ministry of Science and Technology of China
文摘A novel molecularly imprinted polymer (MIP) based on upconversion nanoparticles (UCNPs) was successfully synthesized for determination of Ochratoxin A (OTA). The MIP was developed on the silica-coated UCNPs using N-(1-hydroxy-2-naphthoyl amido)-(L)-phenylalanine (HNA-Phe) as the alternative template. The final composite combined the advantages of the high selectivity of MIP with the high fluorescence intensity of UCNPs which was selective and sensitive to OTA. Under the optimal condition, the fluorescence intensity of UCNPs@SiO2@MIP decreases linearly when the concentration of OTA increases from 0.05 to 1.0 mg/L. The detection limit of OTA with the method was 0.031 mg/L. At three spiked concentration levels (50, 100 and 200 μg/kg), the recovery ranges of OTA in corn, rice and feed are 88.0%–91.6%, 80.2%–91.6% and 89.2%–90.4%, respectively.
基金the funding support from the Singapore Ministry of Education Academic Research Fund (AcRF Tier 3 Grant MOE2016-T3-1-004, R-397-000274-112 AcRF Tier 1 Grant R-397-000-270-114)
文摘Fluorescently encoded microbeads are in demand for multiplexed applications in different fields.Compared to organic dye-based commercially available Luminex's x MAP technology, upconversion nanoparticles(UCNPs) are better alternatives due to their large antiStokes shift, photostability, nil background, and single wavelength excitation. Here, we developed a new multiplexed detection system using UCNPs for encoding poly(ethylene glycol) diacrylate(PEGDA) microbeads as well as for labeling reporter antibody. However, to prepare UCNPs-encoded microbeads, currently used swellingbased encapsulation leads to non-uniformity, which is undesirable for fluorescence-based multiplexing. Hence,we utilized droplet microfluidics to obtain encoded microbeads of uniform size, shape, and UCNPs distribution inside. Additionally, PEGDA microbeads lack functionality for probe antibodies conjugation on their surface.Methods to functionalize the surface of PEGDA microbeads(acrylic acid incorporation, polydopamine coating)reported thus far quench the fluorescence of UCNPs. Here,PEGDA microbeads surface was coated with silica followed by carboxyl modification without compromising the fluorescence intensity of UCNPs. In this study, droplet microfluidics-assisted UCNPs-encoded microbeads of uniform shape, size, and fluorescence were prepared.Multiple color codes were generated by mixing UCNPs emitting red and green colors at different ratios prior to encapsulation. UCNPs emitting blue color were used to label the reporter antibody. Probe antibodies were covalently immobilized on red UCNPs-encoded microbeads for specific capture of human serum albumin(HSA) as a model protein. The system was also demonstrated for multiplexed detection of both human C-reactive protein(hCRP) and HSA protein by immobilizing anti-h CRP antibodies on green UCNPs.
基金supported in part by the National Natural Science Foundation of China(21471043,21304028,51403195,31501576)~~
文摘We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To improve the energy transfer efficiency,UCNPs and CdS nanoparticles were bound in close proximity to each other within the SiO2matrix.β‐NaYF4:Yb(30%),Tm(0.5%)@NaYF4:Yb(20%),Er(2%)core–shell nanoparticles were used as nanotransducers for near infrared light.These nanoparticles exhibited enhanced upconversion fluorescence compared withβ‐NaYF4:Yb(30%),Tm(0.5%)orβ–NaYF4:Yb(30%),Tm(0.5%)@NaYF4nanoparticles.The morphologies,size and chemical compositions have been extensively investigated using field emission scanning electron microscopy(FESEM),transmission electron microscopy(TEM),X‐ray diffraction(XRD)and X‐ray photoelectron spectra(XPS),respectively.The TEM images showed that the TiO2composite nanotubes were embedded with a large amount of UCNPs and CdS nanoparticles.The composite TiO2nanotubes degraded more than90%of rhodamine B(RhB)dye during20min of irradiation by simulated solar light.In particular,more than50%of RhB was decomposed in70min,under irradiation of near infrared light(NIR).This high degradation was attributed to the full spectrum absorption of solar light,and the enhanced transfer efficiency for near infrared light.The as‐prepared nanostructures can harness solar energy,and provide an alternative to overcome energy shortages and environmental protection.
基金This work is partially supported by National Key Research and Development Program of China(Grant No.2018YFC1407503)the Fundamental Research Funds for the Central Universities(2018FZA5001)The National Natural Science Foundation of China(Grant No.11621101).
文摘Two-photon luminescence with near-infrared(NIR)excitation of upconversion nanoparticles(NPs)is of great importance in biological imaging due to deep penetration in high-scattering tissues,low auto-luminescence and good sectioning ability.Unfortunately,common two-photon luminescence is in visible band with an extremely high exciation power density,which limits its application.Here,we synthesized NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs with strong twophoton NIR emission and a low excitation power density.Furthermore,NaYF_(4):Yb/Tm@NaYF_(4)@SiO_(2)@OTMS@F127 NPs with high chemical stability were obtained by a modified multilayer coating method which was applied to upconversion NPs for thefirst time.In addition,it is shown that the as-prepared hydrophillic upconversion NPs have great biocompatibility and kept stable for 6 hours during in vivo whole-body imaging.The vessels with two-photon luminescence were clear even under an excitation power density as low as 25mW/cm^(2).Vivid visualizations of capillaries and vessels in a mouse brain were also obtained with low background and high contrast.Because of cheaper instruments and safer power density,the NIR two-photon luminescence of NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs could promote wider application of two-photon technology.The modified multilayer coating method could be widely used for upconversion NPs to increase the stable time of the in vivo circulation.Our work possesses a great potential for deep imaging and imaging-guided treatment in the future.
基金funded by the National Natural Science Foundation of China(52073131,51902148,61874166,51802024,11974069 and U1832149)the Fundamental Research Funds for the Central Universities(lzujbky-2020-61,lzujbky-2020-64,lzujbky-2021-it31,lzujbky-2021-ct15 and lzujbky-2021-ct01)+2 种基金the Natural Science Foundation of Gansu Province(20JR5RA278 and 20JR5RA24)the LiaoNing Revitalization Talents Program(XLYC1902113)the Science and Technology Program of Qinghai Province(2020-HZ-809)。
文摘To better utilize the infrared(IR)region in sunlight for photovoltaic devices(PVs),upconversion nanoparticles(UCNPs)have been proposed to improve power conversion efficiency(PCE).However,researchers recently have found that the upconversion(UC)effect is negligible in PVs performance improvement for their ultra-low UC photoluminescence quantum yields of UCNPs solid film,while the real mechanism of UCNPs in PVs has not been clearly studied.Herein,based on the material inorganic perovskitesγ-CsPbI_(3),NaYF_(4):20%Yb^(3+),2%Er^(3+)UCNPs were integrated into different transport layer to optimize device performance.Compared with reference device,the short-circuit current density and PCE of optimized device reached 20.87 mA/cm^(2)(20.39 mA/cm^(2))and 18.34%(17.72%),respectively,without sacrificing open-circuit voltage and filling factor.Further experimental characterizations verified that the improved performance was attributable to enhanced visible light absorption instead of IR.To theoretically explain the statement,the light field distribution in device was simulated and the absorption in different layers was calculated.The results revealed that the introduction of UCNPs with different refractive index from other layers caused light field disturbance,and improved visible light captured by γ-CsPbI_(3).Importantly,through experiments and theoretical calculation,the research deeply explored the potential mechanism of UCNPs in optimizing PVs performance.
基金The work was supported by the National Key Research and Development Program of China(YFC20170110100)the National Natural Science Foundation of China(NSFC)(Grant Nos.61475185 and 11504409)Natural Science Foundation of Tianjin City(TJNSF)(Grant No.16JCYBJC43800).Xiaohu Chen and Zhengyu Gui contributed equality to this work.
文摘Luminescent properties of Er^(3+)-and Yb^(3+)-co-doped CaF_(2)upconversion nanoparticles(UCNPs)were investigated in single particle and densely-packed states with a custom-built microscope.The single UCNPs exhibit linear dependency of luminescent intensity on excitation power while the densely-packed UCNPs exhibit a 2-order power law-dependency indicating a two-photon absorption process.Time-domain luminescence intensity measurements were performed and the curves were fitted to excitationnemission rate functions based on a simplified three-state model.The results indicate that the intermediates in single particles are much less and saturated in a short time,and there are strong couplings of the ground states and intermediate states between neighboring UCNPs in densely packed UCNPs.
基金supported by the financial aid from the National Key Research and Development Program of China(No.2021YFF0701800)the National Natural Science Foundation of China(Nos.21871248,21834007,and 22020102003)+2 种基金K.C.Wong Education Foundation(No.GJTD-2018-09)the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.Y201947)Jilin Province Science and Technology Development Plan Project(No.20220101063JC).
文摘Highly toxic reactive oxygen species(ROS)induced apoptosis and ferroptosis have been considered as significant cell death pathways for cancer therapy.However,insufficient amount of intracellular ROS extremely restricts the therapeutic effect.Toward this,we report a rationally designed nanocomposite(mUCC)with enhanced ROS generation ability,inducing the combination of apoptosis and ferroptosis through synergistic photodynamic therapy(PDT)and chemodynamic therapy(CDT).Under 808 nm near-infrared(NIR)light irradiation,photocatalytic reaction is triggered starting from the separation of electron-hole pairs on the surface of heterojunction(CeO_(2)/CuO),realizing improved ROS production.Simultaneously,mUCC served as Fenton-like agent exhibits considerable ability to generate highly toxic·OH under tumor microenvironment(TME).The boosted accumulation of ROS disrupts the redox balance within tumor cells and results in the integration of apoptosis and ferroptosis.In addition,mUCC shows satisfactory tumor targeting property benefiting from the cancer cell membrane functionalization under the guidance of magnetic resonance imaging(MRI)and NIR fluorescence imaging.The intelligent mUCC with good biocompatibility and excellent antitumor response achieves efficient tumor elimination under synergistic PDT and CDT.This work offers an elective approach for further development of ROS-based therapeutic nanoplatform in cancer therapy.
基金This work was supported by the National Natural Science Foundation of China(NSFC)(Nos.U1805252,22175179,22135008,12174392,21975257,and 12104456)NSF of Fujian Province(Nos.2021I0040,2021L3024)the Chinese Academy of Sciences/State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams.
文摘Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing,photocatalysis,anticounterfeiting and nanomedicine.However,precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth mechanisms.Herein,we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites(ZIF-8=zeolitic imidazolate framework-8).The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission,which were verified by steady-state/transient photoluminescence(PL)spectroscopy and single-particle imaging.Ethylenediamine(EDA)was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the composites.By adjusting the concentration of EDA from 0 to 25 mmol/L,the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron(RD)to truncated rhombic dodecahedron(TRD),cube with truncated edges(CTE),cube,and finally a unique form of interpenetration twins(IT).The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy(SEM)images and the formation mechanism was thoroughly revealed.Furthermore,we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and shapes.The proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications.
基金supported by the Science and Technology Development Fund,Macao SAR(Grant 0065/2023/ITP2).
文摘As a widespread element,heavy metals have a significant impact on human health and threaten human health.It is of great significance to develop analytical technologies that can detect heavy metal ions quickly and accurately.In comparison to conventional fluorescent materials such as organic dyes,quantum dot(QD)labels,and carbon quantum dots(CD),fluorescence detection technology utilizing lanthanide(Ln)ion-doped upconversion nanoparticles(UCNPs)stands out due to its distinctive attributes.These include a notably reduced autofluorescence background,enhanced tissue penetration capabilities,biocompatibility with cellular tissues,and minimal photodamage inflicted on biological samples.The utilization of this technology has garnered considerable attention across multiple fields.In the domain of heavy metal detection,traditional laboratory methods necessitate costly instrumentation and a fully equipped laboratory,involving intricate sample processing procedures and protracted detection periods,as well as a demand for skilled personnel.In contrast,the implementation of this material offers rapid and cost-effective detection,significantly mitigating the technical barriers for operators.Consequently,this represents an exceptional avenue to curtail expenses and broaden the scope of detection within the analytical process.This paper reviews the research progress of UCNPs in the detection of heavy metal ions,encompassing a brief elucidation of the luminescence principle of upconversion nanomaterials and commonly used detection principles.Additionally,it provides a detailed overview of the research status of several common non-metal ions and essential heavy metals.Furthermore,it summarizes the current focal points in UCNP detection and discusses the challenges and prospects associated with it.
基金This work was supported by the research start-up fund of Soochow University and the Research Grants Council of Hong Kong SAR(No.CityU5/CRF/08)。
文摘Lanthanide-based upconversion nanoparticles(UCNPs)have been widely explored in various fields,including optical imaging,in recent years.Although earlier work has shown that UCNPs with different lanthanide(Ln3+)dopants exhibit various colors,multicolor-especially in vivo multiplexed biomedical imaging-using UCNPs has rarely been reported.In this work,we synthesize a series of UCNPs with different emission colors and functionalize them with an amphiphilic polymer to confer water solubility.Multicolor in vivo upconversion luminescence(UCL)imaging is demonstrated by imaging subcutaneously injected UCNPs and applied in multiplexed in vivo lymph node mapping.We also use UCNPs for multicolor cancer cell labeling and realize in vivo cell tracking by UCL imaging.Moreover,for the first time we compare the in vivo imaging sensitivity of quantum dot(QD)-based fluorescence imaging and UCNP-based UCL imaging side by side,and find the in vivo detection limit of UCNPs to be at least one order of magnitude lower than that of QDs in our current non-optimized imaging system.Our data suggest that,by virtue of their unique optical properties,UCNPs have great potential for use in highly-sensitive multiplexed biomedical imaging.
基金SVKM's NMIMS University(PhD/20.08.2020)for providing fellowship to carry out research。
文摘Upconversion nanoparticles(UCNPs)doped with lanthanides can convert near-infrared excitation into UV and visible emissions.Because of their relatively high emission efficiency,UCNPs are appealing materials for use in a variety of sectors.UCNPs are known for low auto-fluorescence,excellent chemical and thermal photo-stability,deep tissue penetration,exceptional biocompatibility,low toxicity,color purity,and ease of surface functionalization.In this review,we explain a few recent strategies to boost the efficiency and luminescence of upconversion nanoparticles and minimize quenching by fabricating them as core/shell,nanofibers,or heavily doped lanthanides.Applications of UCNPs in drug delivery,Photodynamic therapy(PDT),biosensors,bioimaging,and optogenetics are also discussed along with their mechanism of action.Our motivation for this review is to understand the working mechanism of UCNPs and their applications in various fields.
基金This work was financially supported by the National Natural Science Foundation of China(Grants 52172276,U20A20379),research fund from Anhui Provincial Institute of Translational Medicine(2021zhyx-B15)Grants for Scientific Research of BSKY(No:XJ201933)from Anhui Medical University.Zhaoyou Chu,Tian Tian,and Zhenchao Tao contributed equally to this work.
文摘UCNPs@AgBiS_(2) core-shell nanoparticles that AgBiS_(2) coated on the surface of upconversion nanoparticles (UCNPs) was successfully prepared through an ion exchange reaction. The photothermal conversion efficiency of AgBiS_(2) can be improved from 14.7% to 45% due to the cross relaxation between Nd ions and AgBiS_(2). The doping concentration of Nd ions played a critical role in the production of reactive oxygen species (ROS) and enhanced the photothermal conversion efficiency. The NaYF4:Yb/Er/Nd@NaYF4:Nd nanoparticles endows strong upcon-version emissions when the doped concentration of Nd ions is 1% in the inner core, which excites the AgBiS_(2) shell to produce ROS for photodynamic therapy (PDT) of cancer cells. As a result, the as-prepared NaYF4:Yb/Er/ Nd@NaYF4:Nd@AgBiS_(2) core-shell nanoparticles showed combined photothermal/photodynamic therapy (PTT/ PDT) against malignant tumors. This work provides an alternative near-infrared light-active multimodal nano-structures for applications such as fighting against cancers.
基金National Natural Science Foundation of China(21905182)Key Research and Development Program of Shandong Province(2019JZZY010355)+3 种基金National Key Research and Development Program of China(2021YFC2101900)Synthetic Leather and High-Performance fibers Innovation Team(2020SCUNG122)615 Talent Introduction Program of Jiangsu Dongtai for Leading TalentsFunda-mental Research Funds for the Central Universities(YJ201940).
文摘Counterfeit leather products infringe the intellectual property rights of the business,cause enormous economic loss,and negatively influence the business enthusiasm for innovation.However,traditional anti-counterfeiting materials for leather products suffer from complicated fabrication procedures,photobleaching,and high volatile organic com-pound(VOC)emissions.Here,a sustainable and invisible anti-counterfeiting ink composed of waterborne polyure-thane and water-dispersible lanthanide-doped upconversion nanoparticles(UCNPs)featuring ease of preparation,high photostability,non-toxicity,low VOC emissions,and strong adhesion strength for leather products is designed and synthesized.After decorating on the surface of leather products,the obtained patterns are invisible under normal light conditions.Upon irradiation at 808 nm,the invisible patterns can be observed by naked eyes due to the visible light emitted by 808 nm excited UCNPs.Our approach described here opens a new pathway to realize the long-term,stable anti-counterfeiting function of leather products.
基金the National Natural Science Foundation of China(No.31860263 to Xiaolei Wang,No.82060095 to Weimin Zhou)Key Youth Project of Jiangxi Province(20202ACB216002 to Xiaolei Wang)+1 种基金Natural Science Foundation of Jiangxi Province(911135755018 to Weimin Zhou)Jiangxi Provincial Graduate Innovation Special Fund(YC2020-B053 to Shichen Liu).
文摘Thromboembolism is the leading cause of cardiovascular mortality.Currently,for the lack of targeting,short half-life,low bioavailability and high bleeding risk of the classical thrombolytic drugs,pharmacological thrombolysis is usually a slow process based on micro-pumping.In addition,frequently monitoring and regulating coagulation functions are also required during(and after)the process of thrombolysis.To address these issues,a targeted thrombolytic and anticoagulation nanoplatform(UCATS-UK)is developed based on upconversion nanoparticles(UCNPs)that can convert 808 or 980 nm near-infrared(NIR)light into UV/blue light.This nanoplatform can target and enrich in the thrombus site.Synergistic thrombolysis and anticoagulation therapy thus could be realized through the controlled release of urokinase(UK)and nitric oxide(NO).Both in vitro and in vivo experiments have confirmed the excellent thrombolytic and anticoagulative capabilities of this multifunctional nanoplatform.Combined with the unique fluorescent imaging capability of UCNPs,this work is expected to contribute to the development of clinical thrombolysis therapy towards an integrated system of imaging,diagnosis and treatment.
基金financial support from the National Natural Science Foundation of China(Nos.22174079,21974073).
文摘Real-time exploring the cellular endocytic pathway of viral capsid proteins(VCPs)functionalized nanocargos at the single-particle level can provide deep insight into the kinetic information involved in virus infection.In this work,porcine circovirus type 2(PCV2)VCPs with different functions are modified onto the surface of upconversion nanoparticles(VCPs-UCNPs)to investigate the cellular internalization process in real-time.Clathrin-mediated endocytosis is found to be the essential uptake mechanism for these VCPs-UCNPs.Besides,it is verified that P_(1)-UCNPs(PCV2 VCPs with nuclear localization signal,namely P1)can be easily assembled close to the perinuclear area,which is different from that of P_(2)-UCNPs(PCV2 VCPs without nuclear localization signal,namely P_(2)).Interestingly,multistep entry processes are observed.Particularly,confined diffusion is observed during the transmembrane process.The intracellular transport of VCPs-UCNPs is dependent on microtubules toward the cell interior.During this process,P_(1)-UCNPs display increased velocities with active transport,while diffusion much faster around the perinuclear area.But for P_(2)-UCNPs,there are only two phases involved in their endocytosis process.This study presents distinct dynamic mechanisms for the nanocargos with different functions,which would make a useful contribution to the development of robust drug delivery systems.
基金Antonios G.Kanaras,Otto L.Muskens and Davide Giust would like to acknowledge funding from BBSRC(Grant No.BB/N021150/1).
文摘We demonstrate the fabrication of a new DNA sensor that is based on the optical interactions occurring between oligonucleotide-coated NaYF4:Yb^(3+);Er^(3+) upconversion nanoparticles and the two-dimensional dichalcogenide materials,MoS_(2) and WS_(2).Monodisperse upconversion nanoparticles were functionalized with single-stranded DNA endowing the nanoparticles with the ability to interact with the surface of the two-dimensional materials via van der Waals interactions leading to subsequent quenching of the upconversion fluorescence.By contrast,in the presence of a complementary oligonucleotide target and the formation of double-stranded DNA,the upconversion nanoparticles could not interact with MoS_(2) and WS_(2),thus retaining their inherent fluorescence properties.Utilizing this sensor we were able to detect target oligonucleotides with high sensitivity and specificity whilst reaching a concentration detection limit as low as 5 mol·L^(-1),within minutes.
基金supported by the National Basic Research Program of China(2016YFA2021600,2016YFA0202104,and2015CB932104)the National Natural Science Foundation of China(31571015,11621505,and 21320102003)Chinese Academy of Sciences Youth Innovation Promotion Association(2013007)
文摘Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 nm irradiation. The application of 808 nm laser as the excitation source could achieve better penetration depth and avoid overheating problem. The combination of UCNPs and RBS could realize the on-demand release of NO at desired time and location by simply controlling the output of NIR laser.Cellular uptake results showed that more nanoparticles were internalized in cancer stem-like cells(CSCs)rather than non-CSCs. Therefore, a synergistic cancer therapy strategy to eradicate both CSCs and nonCSCs simultaneously was developed. Traditional chemo-drug could inhibit non-CSCs but has low killing efficiency in CSCs. However, we found that the combination of NO and chemotherapy could efficiently inhibit CSCs in bulk cells, including inhibiting mammosphere formation ability, decreasing CD44^+/CD24^- subpopulation and reducing tumorigenic ability. The mechanism studies confirmed that NO could not only induce apoptosis but also increase drug sensitivity by declining drug efflux in CSCs. This UCNPsbased platform may provide a new combinatorial strategy of NO and chemotherapy to improve cancer treatment.
基金Science and Technology Innovation Commission of Shenzhen(KQTD20170810110913065,20200925174735005)Australia China Science and Research Fund Joint Research Centre for Point-of-Care Testing(ACSRF658277,SQ2017YFGH001190)ARC Laureate Fellowship Program(D.J.,FL210100180)。
文摘Although small EVs(sEVs)have been used widely as biomarkers in disease diagnosis,their heterogeneity at single EV level has rarely been revealed.This is because high-resolution characterization of sEV presents a major challenge,as their sizes are below the optical diffraction limit.Here,we report that upconversion nanoparticles(UCNPs)can be used for super-resolution profiling the molecular heterogeneity of sEVs.We show that Er3+-doped UCNPs has better brightness and Tm3+-doped UCNPs resulting in better resolution beyond diffraction limit.Through an orthogonal experimental design,the specific targeting of UCNPs to the tumour epitope on single EV has been cross validated,resulting in the Pearson’s R-value of 0.83 for large EVs and~65%co-localization double-positive spots for sEVs.Furthermore,super-resolution nanoscopy can distinguish adjacent UCNPs on single sEV with a resolution of as high as 41.9 nm.When decreasing the size of UCNPs from 40 to 27 nm and 18 nm,we observed that the maximum UCNPs number on single sEV increased from 3 to 9 and 21,respectively.This work suggests the great potentials of UCNPs approach“digitally”quantify the surface antigens on single EVs,therefore providing a solution to monitor the EV heterogeneity changes along with the tumour progression progress.
基金supported by the National Natural Science Foundation of China(21003013)the Jilin Province Science and Technology Development Project(No.20170101094JC)the Scientific Research Fund of Jilin Provincial Education Department (2016323)
文摘Multimodal imaging nanoprobes are urgently sought because they can integrate different imaging func- tion into individual nanoplatform and provide more comprehensive and accurate information for the diagnosis of early-stage tumor. Lanthanide-based upconversion nanoparticles (UCNPs) are regarded as promising nanoplatforms to fabricate these probes. Herein, we firstly developed the active core-active shell structured NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs with the average diameter of 13.23 + 0.96 nm as multimodal imaging probes. These water-dispersible nanoprobes presented excellent near-infrared to near-infrared (NIR-to-NIR) upconversion luminescence (UCL) performance, which is favorable for optical bioimaging due to deeper tissue penetration and autofluorescence reduction. After coated with the NaGdF4:Yb active shell, the UCL emission intensity at 800 nm increased by 7.2 times. These nanoprobes exhibited a desirable longitudinal relaxivity (rl = 3.58 L/(mmol s)) and strong X-ray attenuation property (58.84 HU L/g). The cytotoxicity assessment, histology analysis and biodistribution study revealed that NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs had relatively low cytotoxicity and negligible organ toxicity. These UCNPs were applied for NIR-to-NIR UCL imaging in vivo. More importantly, the detection of small tumor was successfully achieved under Trweighted MRI and CT imaging modalities after intravenous injection of these UCNPs. These results revealed that NaYbF4:Tm@NaGdF4:Yb-PVP UCNPs could serve as promising NIR-to-NIR UCL/MRI/CT trimodal imaging probes.
基金the Ministry of Science and Higher Education within the State assignment FSRC《Crystallography and Photonics》RAS in part of《UCNP synthesis》,by the Russian Foundation for Basic Research according to the research projects No 18-29-20064 in the part of《PL analysis》and Ns 20-32-70174 in the part o f《complex structures analysis》,by the Russian Science Foundation project No18-79-10198 in the part of《UCNP analysis》.BC acknowledges financial support from Lower Saxony through“Quanten und Nanometrologie”project(QUANOMET)and DFG Cluster of Excellence PhoenixD(EXC 2122,Project ID 390833453).
文摘One dimensional(1D)nanostructures attract considerable attention,enabling a broad application owing to their unique properties.However,the precise mechanism of 1D morphology attainment remains a matter of debate.In this study,ultrafast picosecond(ps)laser-induced treatment on upconversion nanoparticles(UCNPs)is offered as a tool for 1 D-nanostructures formation.Fragmentation,reshaping through recrystallization process and bioadaptation of initially hydrophobic(β-Na_(1.5)Y_(1.5_)F_(6):Yb^(3+),Tm^(3+)/β-Na_(1.5)Y_(1.5_)F_(6))core/shell nanoparticles by means of one-step laser treatment in water are demonstrated.“True”1D nanostructures through"Medusa^-like structures can be obtained,maintaining anti-Stokes luminescence functionalities.A matter of the one-dimensional UCNPs based on direction of energy migration processes is debated.The proposed laser treatment approach is suitable for fast UCNP surface modification and nano-to-nano transformation,that open unique opportunities to expand UCNP applications in industry and biomedicine.