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1.
Here a multifunctional nanoplatform (upconversion nanoparticles (UCNPs)‐platinum(IV) (Pt(IV))?ZnFe2O4, denoted as UCPZ) is designed for collaborative cancer treatment, including photodynamic therapy (PDT), chemotherapy, and Fenton reaction. In the system, the UCNPs triggered by near‐infrared light can convert low energy photons to high energy ones, which act as the UV–vis source to simultaneously mediate the PDT effect and Fenton's reaction of ZnFe2O4 nanoparticles. Meanwhile, the Pt(IV) prodrugs can be reduced to high virulent Pt(II) by glutathione in the cancer cells, which can bond to DNA and inhibit the copy of DNA. The synergistic therapeutic effect is verified in vitro and in vivo results. The cleavage of Pt(IV) from UCNPs during the reduction process can shift the larger UCPZ nanoparticles (NPs) to the smaller ones, which promotes the enhanced permeability and retention (EPR) and deep tumor penetration. In addition, due to the inherent upconversion luminescence (UCL) and the doped Yb3+ and Fe3+ in UCPZ, this system can serve as a multimodality bioimaging contrast agent, covering UCL, X‐ray computed tomography, magnetic resonance imaging, and photoacoustic. A smart all‐in‐one imaging‐guided diagnosis and treatment system is realized, which should have a potential value in the treatment of tumor.  相似文献   

2.
Upconverting nanoparticles (UCNPs) have attracted considerable attention as potential photosensitizer carriers for photodynamic therapy (PDT) in deep tissues. In this work, a new and efficient NIR photosensitizing nanoplatform for PDT based on red‐emitting UCNPs is designed. The red emission band matches well with the efficient absorption bands of the widely used commercially available photosensitizers (Ps), benefiting the fluorescence resonance energy transfer (FRET) from UCNPs to the attached photosensitizers and thus efficiently activating them to generate cytotoxic singlet oxygen. Three commonly used photosensitizers, including chlorine e6 (Ce6), zinc phthalocyanine (ZnPc) and methylene blue (MB), are loaded onto the alpha‐cyclodextrin‐modified UCNPs to form Ps@UCNPs complexes that efficiently produce singlet oxygen to kill cancer cells under 980 nm near‐infrared excitation. Moreover, two different kinds of drugs are co‐loaded onto these nanoparticles: chemotherapy drug doxorubicin and PDT agent Ce6. The combinational therapy based on doxorubicin (DOX)‐induced chemotherapy and Ce6‐triggered PDT exhibits higher therapeutic efficacy relative to the individual means for cancer therapy in vitro.  相似文献   

3.
DNA‐mediated assembly of core–satellite structures composed of Zr(IV)‐based porphyrinic metal‐organic framework (MOF) and NaYF4,Yb,Er upconverting nanoparticles (UCNPs) for photodynamic therapy (PDT) is reported. MOF NPs generate singlet oxygen (1O2) upon photoirradiation with visible light without the need for additional small molecule, diffusional photosensitizers such as porphyrins. Using DNA as a templating agent, well‐defined MOF–UCNP clusters are produced where UCNPs are spatially organized around a centrally located MOF NP. Under NIR irradiation, visible light emitted from the UCNPs is absorbed by the core MOF NP to produce 1O2 at significantly greater amounts than what can be produced from simply mixing UCNPs and MOF NPs. The MOF–UCNP core–satellite superstructures also induce strong cell cytotoxicity against cancer cells, which are further enhanced by attaching epidermal growth factor receptor targeting affibodies to the PDT clusters, highlighting their promise as theranostic photodynamic agents.  相似文献   

4.
Multifunctional nanoparticles are synthesized for both pH‐triggered drug release and imaging with radioluminescence, upconversion luminescent, and magnetic resonance imaging (MRI). The particles have a yolk‐in‐shell morphology, with a radioluminescent core, an upconverting shell, and a hollow region between the core and shell for loading drugs. They are synthesized by controlled encapsulation of a radioluminescent nanophosphor yolk in a silica shell, partial etching of the yolk in acid, and encapsulation of the silica with an upconverting luminescent shell. Metroxantrone, a chemotherapy drug, was loaded into the hollow space between X‐ray phosphor yolk and up‐conversion phosphor shell through pores in the shell. To encapsulate the drug and control the release rate, the nanoparticles are coated with pH‐responsive biocompatible polyelectrolyte layers of charged hyaluronic acid sodium salt and chitosan. The nanophosphors display bright luminescence under X‐ray, blue light (480 nm), and near infrared light (980 nm). They also served as T1 and T2 MRI contrast agents with relaxivities of 3.5 mM?1 s?1 (r1) and 64 mM?1s?1 (r2). These multifunctional nanocapsules have applications in controlled drug delivery and multimodal imaging.  相似文献   

5.
Nanomaterials have gained considerable attention and interest in the development of novel and high‐resolution contrast agents for medical diagnosis and prognosis in clinic. A classical urea‐based homogeneous precipitation route that combines the merits of in situ thermal decomposition and surface modification is introduced to construct polyethylene glycol molecule (PEG)‐decorated hybrid lutetium oxide nanoparticles (PEG–UCNPs). By utilizing the admirable optical and magnetic properties of the yielded PEG–UCNPs, in vivo up‐conversion luminescence and T1‐enhanced magnetic resonance imaging of small animals are conducted, revealing obvious signals after subcutaneous and intravenous injection, respectively. Due to the strong X‐ray absorption and high atomic number of lanthanide elements, X‐ray computed‐tomography imaging based on PEG–UCNPs is then designed and carried out, achieving excellent imaging outcome in animal experiments. This is the first example of the usage of hybrid lutetium oxide nanoparticles as effective nanoprobes. Furthermore, biodistribution, clearance route, as well as long‐term toxicity are investigated in detail after intravenous injection in a murine model, indicating the overall safety of PEG–UCNPs. Compared with previous lanthanide fluorides, our nanoprobes exhibit more advantages, such as facile construction process and nearly total excretion from the animal body within a month. Taken together, these results promise the use of PEG–UCNPs as a safe and efficient nanoparticulate contrast agent for potential application in multimodal imaging.  相似文献   

6.
Developing an effective theranostic nanoplatform remains a great challenge for cancer diagnosis and treatment. Here, BiOI@Bi2S3@BSA (bovine serum albumin) semiconductor heterojunction nanoparticles (SHNPs) for triple‐combination radio/photodynamic/photothermal cancer therapy and multimodal computed tomography/photoacoustic (CT/PA) bioimaging are reported. On the one hand, SHNPs possess strong X‐ray attenuation capability since they contain high‐Z elements, and thus they are anticipated to be a very competent candidate as radio‐sensitizing materials for radiotherapy enhancement. On the other hand, as a semiconductor, the as‐prepared SHNPs offer an extra approach for reactive oxygen species generation based on electron–hole pair under the irradiation of X‐ray through the photodynamic therapy process. This X‐ray excited photodynamic therapy obviously has better penetration depth in bio‐tissue. What's more, the SHNPs also possess well photothermal conversion efficiency for photothermal therapy, because Bi2S3 is a thin band semiconductor with strong near‐infrared absorption that can cause local overheat. In vivo tumor ablation studies show that synergistic radio/photodynamic/photothermal therapy achieves more significant therapeutic effect than any single treatment. In addition, with the strong X‐ray attenuation and high near‐infrared absorption, the as‐obtained SHNPs can also be applied as a multimodal contrast agent in CT/PA imaging.  相似文献   

7.
Near infrared (NIR) light triggered phototherapy including photothermal therapy (PTT) and photodynamic therapy (PDT) affords superior outcome in cancer treatment. However, the reactive oxygen species (ROS) generated by NIR‐excited upconversion nanostructure is limited by the feeble upconverted light which cannot activate PDT agents efficiently. Here, an IR‐808 dye sensitized upconversion nanoparticle (UCNP) with a chlorin e6 (Ce6)‐functionalized silica layer is developed for PDT agent. The two booster effectors (dye‐sensitization and core–shell enhancement) synergistically amplify the upconversion efficiency, therefore achieving superbright visible emission under low 808 nm light excitation. The markedly amplified red light subsequently triggers the photosensitizer (Ce6) to produce large amount of ROS for efficient PDT. After the silica is endowed with positive surface, these PDT nanoparticles can be easily grafted on MoS2 nanosheet. As the optimal laser wavelength of UCNPs is consistent with that of MoS2 nanosheet for PTT, the invented nanoplatform generates both abundant ROS and local hyperthermia upon a single 808 nm laser irradiation. Both the in vitro and in vivo assays validate that the innovated nanostructure presents excellent cancer cell inhibition effectiveness by taking advantages of the synergistic PTT and PDT, simultaneously, posing trimodal (upconversion luminescence/computed tomography (CT)/magnetic resonance imaging (MRI) imaging capability.  相似文献   

8.
The increasing uses of rare‐earth‐doped upconversion nanoparticles (UCNPs) have obviously caused many concerns about their potential toxicology on live organisms. In addition, the UCNPs can be released into the environment, then transported into edible crop plants, and finally entered into food chain. Here, the soybean is chosen as a model plant to study the subchronic phytotoxicity, translocation, and biotransformation of NaYF4 UCNPs. The incubation with UCNPs at a relative low concentration of 10 μg mL?1 leads to growth promotion for the roots and stems, while concentration exceeding 50 μg mL?1 brings concentration‐dependent inhibition. Upconversion luminescence imaging and scanning electron microscope characterization show that the UCNPs can be absorbed by roots and parts of the adsorbed UCNPs are then transported through vessels to stems and leaves. The near‐edge X‐ray absorption fine structure spectra reveal that the adsorbed NaYF4 nanoparticles are relatively stable during a 10 d incubation. Energy‐dispersive X‐ray spectrum further indicates that a small amount of NaYF4 is dissolved/digested and can transform into Y‐phosphate clusters in roots.  相似文献   

9.
The luminous efficiency of inorganic white light‐emitting diodes, to be used by the next generation as light initiators, is continuously progressing and is an emerging interest for researchers. However, low color‐rendering index (Ra), high correlated color temperature (CCT), and poor stability limit its wider application. Herein, it is reported that Sm3+‐ and Eu3+‐doped calcium scandate (CaSc2O4 (CSO)) are an emerging deep‐red‐emitting material with promising light absorption, enhanced emission properties, and excellent thermal stability that make it a promising candidate with potential applications in emission display, solid‐state white lighting, and the device performance of perovskite solar cells (PSCs). The average crystal structures of Sm3+‐doped CSO are studied by synchrotron X‐ray data that correspond to an extremely rigid host structure. Samarium ion is incorporated as a sensitizer that enhances the emission intensity up to 30%, with a high color purity of 88.9% with a 6% increment. The impacts of hosting the sensitizer are studied by quantifying the lifetime curves. The CaSc2O4:0.15Eu3+,0.03Sm3+ phosphor offers significant resistance to thermal quenching. The incorporation of lanthanide ion‐doped phosphors CSOE into PSCs is investigated along with their potential applications. The CSOE‐coated PSCs devices exhibit a high current density and a high power conversion efficiency (15.96%) when compared to the uncoated control devices.  相似文献   

10.
Developing high‐voltage cathode materials is critical for sodium‐ion batteries to boost energy density. NASICON (Na super‐ionic conductor)‐structured NaxMnM(PO4)3 materials (M represents transition metal) have drawn increasing attention due to their features of robust crystal framework, low cost, as well as high voltage based on Mn4+/Mn3+ and Mn3+/Mn2+ redox couples. However, full activation of Mn4+/Mn3+ redox couple within NASICON framework is still a great challenge. Herein, a novel NASICON‐type Na4MnCr(PO4)3 material with highly reversible Mn4+/Mn3+ redox reaction is discovered. It proceeds a two‐step reaction with voltage platforms centered at 4.15 and 3.52 V versus Na+/Na, delivering a capacity of 108.4 mA h g?1. The Na4MnCr(PO4)3 cathode also exhibits long durability over 500 cycles and impressive rate capability up to 10 C. The galvanostatic intermittent titration technique (GITT) test shows fast Na diffusivity which is further verified by density functional theory calculations. The high electrochemical activity derives from the 3D robust framework structure, fast kinetics, and pseudocapacitive contribution. The sodium storage mechanism of the Na4MnCr(PO4)3 cathode is deeply studied by ex situ X‐ray diffraction (XRD) and ex situ X‐ray photoelectron spectroscopy (XPS), revealing that both solid‐solution and two‐phase reactions are involved in the Na+ ions extraction/insertion process.  相似文献   

11.
Inspired by its high‐active and open layered framework for fast Li+ extraction/insertion reactions, layered Ni‐rich oxide is proposed as an outstanding Na‐intercalated cathode for high‐performance sodium‐ion batteries. An O3‐type Na0.75Ni0.82Co0.12Mn0.06O2 is achieved through a facile electrochemical ion‐exchange strategy in which Li+ ions are first extracted from the LiNi0.82Co0.12Mn0.06O2 cathode and Na+ ions are then inserted into a layered oxide framework. Furthermore, the reaction mechanism of layered Ni‐rich oxide during Na+ extraction/insertion is investigated in detail by combining ex situ X‐ray diffraction, X‐ray photoelectron spectroscopy, and electron energy loss spectroscopy. As an excellent cathode for Na‐ion batteries, O3‐type Na0.75Ni0.82Co0.12Mn0.06O2 delivers a high reversible capacity of 171 mAh g?1 and a remarkably stable discharge voltage of 2.8 V during long‐term cycling. In addition, the fast Na+ transport in the cathode enables high rate capability with 89 mAh g?1 at 9 C. The as‐prepared Ni‐rich oxide cathode is expected to significantly break through the limited performance of current sodium‐ion batteries.  相似文献   

12.
The advancements in nanotechnology have created multifunctional nanomaterials aimed at enhancing diagnostic accuracy and treatment efficacy for cancer. However, the ability to target deep‐seated tumors remains one of the most critical challenges for certain nanomedicine applications. To this end, X‐ray‐excited theranostic techniques provide a means of overcoming the limits of light penetration and tissue attenuation. Herein, a comprehensive overview of the recent advances in nanotechnology‐enhanced X‐ray‐excited imaging and therapeutic methodologies is presented, with an emphasis on the design of multifunctional nanomaterials for contrast‐enhanced computed tomography (CT) imaging, X‐ray‐excited optical luminescence (XEOL) imaging, and X‐ray‐excited multimodal synchronous/synergistic therapy. The latter is based on the concurrent use of radiotherapy with chemotherapy, gas therapy, photodynamic therapy, or immunotherapy. Moreover, the featured biomedical applications of X‐ray‐excited deep theranostics are discussed to highlight the advantages of X‐ray in high‐sensitivity detection and efficient elimination of malignant tumors. Finally, key issues and technical challenges associated with this deep theranostic technology are identified, with the intention of advancing its translation into the clinic.  相似文献   

13.
Readily commercializable and cost‐effective next‐generation CsPbBr3 perovskite nanocrystals (PNCs) based X‐ray detectors are demonstrated. The PNCs‐based X‐ray detector exhibits higher spatial resolution (9.8 lp mm?1 at modulation transfer function (MTF) = 0.2 and 12.5–8.9 lp mm?1 for a linear line chart), faster response time (≈200 ns), and comparable stability (>40 Gyair s?1 of X‐ray exposure) compared with the commercialized terbium‐doped gadolinium oxysulfide (GOS)‐based detectors (spatial resolution = 6.2 lp mm?1 at MTF = 0.2 and 6.3 lp mm?1 for a linear line chart, response time = ≈1200 ns) because the PNCs‐based scintillator has ≈5.6‐fold faster average photoluminescence lifetime and stronger emission than the GOS‐based one.  相似文献   

14.
The discovery of high efficiency narrow‐band green‐emitting phosphors is a major challenge in backlighting light‐emitting diodes (LEDs). Benefitting from highly condensed and rigid framework structure of UCr4C4‐type compounds, a next‐generation narrow green emitter, RbLi(Li3SiO4)2:Eu2+ (RLSO:Eu2+), has emerged in the oxide‐based family with superior luminescence properties. RLSO:Eu2+ phosphor can be efficiently excited by GaN‐based blue LEDs, and shows green emission at 530 nm with a narrow full width at half maximum of 42 nm, and very low thermal quenching (103%@150 °C of the integrated emission intensity at 20 °C), however its chemical stability needs to be improved later. The white LED backlight using optimized RLSO:8%Eu2+ phosphor demonstrates a high luminous efficacy of 97.28 lm W?1 and a wide color gamut (107% National Television System Committee standard (NTSC) in Commission Internationale de L'Eclairage (CIE) 1931 color space), suggesting its great potential for industrial applications as liquid crystal display (LCD) backlighting.  相似文献   

15.
To improve the energy and power density of Na‐ion batteries, an increasing number of researchers have focused their attention on activation of the anionic redox process. Although several materials have been proposed, few studies have focused on the Na‐rich materials compared with Li‐rich materials. A key aspect is sufficient utilization of anionic species. Herein, a comprehensive study of Mn‐based Na1.2Mn0.4Ir0.4O2 (NMI) O3‐type Na‐rich materials is presented, which involves both cationic and anionic contributions during the redox process. The single‐cation redox step relies on the Mn3+/Mn4+, whereas Ir atoms build a strong covalent bond with O and effectively suppress the O2 release. In situ Raman, ex situ X‐ray photoelectron spectroscopy, and soft‐X‐ray absorption spectroscopy are employed to unequivocally confirm the reversibility of O22? species formation and suggest a high degree of anionic reaction in this NMI Na‐rich material. In operando X‐ray diffraction study discloses the asymmetric structure evolution between the initial and subsequent cycles, which also explains the effect of the charge compensation mechanism on the electrochemical performance. The research provides a novel insight on Na‐rich materials and a new perspective in materials design towards future applications.  相似文献   

16.
Upconversion nanoparticles (UCNPs) doped with lanthanide ions that possess ladder-like energy levels can give out multiple emissions at specific ultra-violet or visible wavelengths irrespective of excitation light. However, precisely controlling energy migration processes between different energy levels of the same lanthanide ion to generate switchable emissions remains elusive. Herein, a novel dumbbell-shaped UCNP is reported with upconverted red emission switched to green emission when excitation wavelength changed from 980 to 808 nm. The sensitizer Yb ions are doped with activator Er ions and energy modulator Mn ions in NaYF4 core nanocrystal coated with an inner NaYF4:Yb shell to generate red emission after harvesting 980 nm excitation light, while an outer NaNdF4:Yb shell is coated to form a dumbbell shape to generate green emission upon 808 nm excitation. Such specially designed UCNPs with switchable green and red emissions are further explored for imaging of latent fingerprint and detection of explosive residues in the fingerprint simultaneously. This work suggests a novel research interest in fine-tuning of upconversion emissions through precisely controlling energy migration processes of the same lanthanide activator ion. Furthermore, use of these nanoparticles in other applications such as simultaneous dual-color imaging or orthogonal bidirectional photoactivation can be explored.  相似文献   

17.
Sonodynamic therapy (SDT) triggered by ultrasound (US) has attracted increasing attention owing to its abilities to overcome critical limitations including low tissue‐penetration depth and phototoxicity in photodynamic therapy. Herein, the design of a new type of sonosensitizer is revealed, namely, ultrasmall oxygen‐deficient bimetallic oxide MnWOX nanoparticles, for multimodal imaging‐guided enhanced SDT against cancer. As‐made MnWOX nanoparticles with poly(ethylene glycol) (PEG) modification show high physiological stability and biocompatibility. Interestingly, such MnWOX‐PEG nanoparticles exhibit highly efficient US‐triggered production of 1O2 and ?OH, higher than that of previously reported sonosensitizers (e.g., protoporphyrin IX and titanium dioxide), because the oxygen‐deficient structure of MnWOX serves as an electron trap site to prevent electron–hole recombination. The glutathione depletion capability of MnWOX‐PEG can also further favor SDT‐triggered cancer cell killing. With efficient tumor homing as illustrated by computer tomography and magnetic resonance imaging, MnWOX‐PEG enables effective destruction of mouse tumors under US stimulation. After accomplishing its therapeutic functions, MnWOX‐PEG can be metabolized by the mouse body without any long‐term toxicity. Herein, a new type of sono‐sensitizing agent with high SDT efficacy, multimodal imaging functions, and rapid clearance is presented, an agent which is promising for noninvasive SDT cancer treatment.  相似文献   

18.
Chromium‐doped zinc gallate, ZnGa2O4:Cr3+ (ZGC), is viewed as a long‐lasting luminescence (LLL) phosphor that can avoid tissue autofluorescence interference for in vivo imaging detection. ZGC is a cubic spinel structure, a typical agglomerative or clustered morphology lacking a defined cubic shape, but a sphere‐like feature is commonly obtained for the nanometric ZGC. The substantial challenge remains achieving a well‐defined cubic feature in nanoscale. The process by which dispersed and well‐defined concave cubic ZGC is obtained is described, exhibiting much stronger LLL in UV and X‐ray excitation for the dispersed cubic ZGC compared with the agglomerative form that cannot be excited using X‐rays with a low dose of 0.5 Gy. The cubic ZGC reveals a specific accumulation in liver and 0.5 Gy used at the end of X‐ray excitation is sufficient for imaging of deep‐seated hepatic tumors. The ZGC nanocubes show highly passive targeting of orthotopic hepatic tumors.  相似文献   

19.
A series of polycrystalline Na4Ca4(Si6O18):Eu3+ orange emitting phosphors were synthesized by a conventional high-temperature solid-state reaction. The phase formation was confirmed by X-ray power diffraction analysis. The excitation spectra show a strong host absorption indicating an efficient energy transfer process from O2? to Eu3+ ions. Upon NUV radiation, the phosphors showed strong red emission around 610 nm (5D0 → 7F2) and orange emission around 591 nm (5D0 → 7F1), but the 5D1,2,3 emission nearly can not be seen. Compared with the luminescence properties of Li+, Na+, and K+ co-doped samples, we deduced that Na+ ions probably prefer to dope into the intrinsic Na vacancies rather than Ca2+ ions vacancies in Na4Ca4(Si6O18) crystal. Thermal stability properties, quantum efficiency and chromaticity coordinates of the phosphors have been investigated for the potential application in white LEDs.  相似文献   

20.
An alternative routine is presented by constructing a novel architecture, conductive metal/transition oxide (Co@Co3O4) core–shell three‐dimensional nano‐network (3DN) by surface oxidating Co 3DN in situ, for high‐performance electrochemical capacitors. It is found that the Co@Co3O4 core–shell 3DN consists of petal‐like nanosheets with thickness of <10 nm interconnected forming a 3D porous nanostructure, which preserves the original morphology of Co 3DN well. X‐ray photoelectron spectroscopy by polishing the specimen layer by layer reveals that the Co@Co3O4 nano‐network is core–shell‐like structure. In the application of electrochemical capacitors, the electrodes exhibit a high specific capacitance of 1049 F g?1 at scan rate of 2 mV/s with capacitance retention of ~52.05% (546 F g?1 at scan rate of 100 mV) and relative high areal mass density of 850 F g?1 at areal mass of 3.52 mg/cm2. It is believed that the good electrochemical behaviors mainly originate from its extremely high specific surface area and underneath core‐Co “conductive network”. The high specific surface area enables more electroactive sites for efficient Faradaic redox reactions and thus enhances ion and electron diffusion. The underneath core‐Co “conductive network” enables an ultrafast electron transport.  相似文献   

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