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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Achieving a “all in one” Fe/Tm-MOFs with controllable photothermal and catalytic performance for imaging-guided multi-modal synergetic therapy

Haiqing Gao,Qin Ji,Bin Chi,Caixue Lin,Gang Ding,Yingxi Wang,Xiaolan Yu,Zushun Xu,Run Zhang,Ling Li,Jing Wang

Targeting excess H 2 O 2 in the tumor microenvironment, nanotheranostic agents for catalytic therapy are designed based on Fenton reaction, catalyzing H 2 O 2 into oxygen and hydroxyl radical ( OH). But the catalytic efficiency in tumor microenvironment is not satisfactory. In order to solve the problem, a series of bimetallic-dual ligands metal-organic frameworks Fe/Tm-MOFs were designed, that Fe 3+ and Tm 3+ as metalions, 2-methylimidazole and trimesic acid as ligands. Due to the doped Tm 3+ in Fe/Tm-MOFs and the conjugated structures formed by two ligands, the rate of electron transfer was improved, thus promoting the generation of OH at some extent. In addition, the photothermal effect of Fe/Tm-MOFs further promotes the generation of OH, which was evidenced by the 3,3′,5,5′-tetramethylbenzidine(TMB). Combining the drug loading and release capabilities of Fe/Tm-MOFs, synergetic therapy of photothermal/chemo-/catalytic therapy can be achieved. In vitro results reveal that DOX release behaviors are both pH- and thermal-responsive. In vivo anti-cancer results show that the tumors of mice almost disappeared within 10 days, which were injected with Fe/Tm-MOFs/DOX and irradiated with 808 nm for 10 min. Thus, an excellent therapeutic performance has been achieved. Besides, Fe/Tm-MOFs can serve as a multimodality bioimaging contrast agent, covering fluorescence imaging, photothermal imaging and magnetic resonance imaging. Thus, an all-in-one nanotheranostic agent is constructed, improving the catalytic efficiency and providing a novel method to design an efficient nanotheranostic agent.

研究领域: 生物医学工程 · 纳米医学 · 肿瘤学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2017 ·Vol. 19 ·期 47 ·31675-31683 · IF 4.123

Optical–magnetic bifunctional properties and mechanistic insights on upconversion of NaYF4:Yb,Ho,Tm@NaGdF4 with a tunable nanodumbbell morphology

Zhichao Yu,Haifeng Zhou,Guangjun Zhou,Juan Zhou,Yaqiang Wu,Xingshuang Zhang,Tao Wang,Dapeng Huang,Xinqiang Wang,Jifan Hu

The energy-upconversion of lanthanide-doped nanoparticles with a core–shell structure can be utilized to enhance and tune optical properties and can generate multifunctionality in a single system. Herein, the core–shell nanoparticles NaYF4:Yb,Ho,Tm@NaGdF4 were prepared by thermally decomposing lanthanide acetylacetonate precursors. Through modifying the molar ratio of the core and shell, nanodumbbell-shaped particles with different sizes and morphologies were precisely synthesized. The formation mechanism and the heterogeneous epitaxial growth process of the nanodumbbell-shaped particles were studied. After coating the shell layer, upconversion luminescence intensities, spectral purity and fluorescence lifetimes were improved. Furthermore, the magnetic performance of the core–shell nanoparticles was characterized. The optical–magnetic bifunctional upconversion core–shell particles with programmable shape and multiple properties provide an ideal platform for the preparation of nanodumbbell-shaped particles and the promotion of upconversion materials for biomedical research.

研究领域: 材料科学 · 生物医学工程 · 纳米技术
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FOOD CHEMISTRY · 2021 · IF 7.514

Quantitative image analysis method for detection of nitrite with cyanine dye-NaYF4:Yb,Tm@NaYF4 upconversion nanoparticles composite luminescent probe

Hongqi Chen,Wei Tang,Yunchun Liu,Lun Wang

In this work, a quantitative image analysis method based on cyanine dye-upconversion nanoparticles composite luminescent nanoprobe for the detection of nitrite was developed. The nanoprobe was constructed by combining the NaYF 4 :Yb,Tm@NaYF 4 upconversion nanoparticles (UCNPs) and the new cyanine dye IR-790. The upconversion nanoparticles transferred energy to IR-790, resulting in the luminescence quenching, while the luminescence of UCNPs was recovered after adding NO 2 − . The increase in photons was related to the concentration of NO 2 − . Under the optimal experimental conditions, the detection range was 0.20–140 μM and the limit of detection was 0.030 μM. The measurement for NO 2 − can be completed in 29 min. The method has the characteristics of fast response (~0.1 s), low sample consumption (10 μL) and powerful data support (550 frame time series images). Furthermore, the quantitative image analysis method was successfully applied for the analysis of nitrite in environmental water and food samples.

研究领域: 分析化学 · 环境科学 · 食品科学
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BIOMATERIALS · 2015 · IF 8.557

Doxorubicin-loaded NaYF4:Yb/Tm–TiO2 inorganic photosensitizers for NIR-triggered photodynamic therapy and enhanced chemotherapy in drug-resistant breast cancers

Leyong Zeng,Yuanwei Pan,Ying Tian,Xin Wang,Wenzhi Ren,Shouju Wang,Guangming Lu,Aiguo Wu

The combination therapy has exhibited important potential for the treatment of cancers, especially for drug-resistant cancers. In this report, bi-functional nanoprobes based on doxorubicin (DOX)-loaded NaYF 4 :Yb/Tm–TiO 2 inorganic photosensitizers (FA-NPs-DOX) were synthesized for in vivo near infrared (NIR)-triggered inorganic photodynamic therapy (PDT) and enhanced chemotherapy to overcome the multidrug resistance (MDR) in breast cancers. Using the up-conversion luminescence (UCL) performance of NaYF 4 :Yb/Tm converting near-infrared (NIR) into ultraviolent (UV) lights, reactive oxygen species (ROS) were triggered from TiO 2 inorganic photosensitizers for PDT under the irradiation of a 980 nm laser, by which the deep-penetration and low photo-damage could be reached. Moreover, nanocarrier delivery and folic acid (FA) targeting promoted the cellular uptake, and accelerated the release of DOX in drug-sensitive MCF-7 and resistant MCF-7/ADR cells. The toxicity assessment in vitro and in vivo revealed the good biocompatibility of the as-prepared FA-NPs-DOX nanocomposites . By the combination of enhanced chemotherapy and NIR-triggered inorganic PDT, the viability of MCF-7/ADR cells could decrease by 53.5%, and the inhibition rate of MCF-7/ADR tumors could increase up to 90.33%, compared with free DOX. Therefore, the MDR of breast cancers could be obviously overcome by enhanced chemotherapy and NIR-triggered inorganic PDT of FA-NPs-DOX nanocomposites under the excitation of a 980 nm laser.

研究领域: 肿瘤学 · 纳米医学 · 生物材料学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 10 ·4806-4813 · IF 3.925

Near-infrared light-triggered β-NaYF4:Yb,Tm,Gd@MIL-100(Fe) nanomaterials for antibacterial applications

Jie Song,Leilei Sun,Hongchao Geng,Wenlong Tan,Deshuai Zhen,Qingyun Cai

β-Phase NaYF4:Yb,Tm,Gd up-conversion nanorods (UCNRs) with high uniformity were synthesized by a solvothermal method. The optimal fluorescence intensity of UCNRs was explored. After further modification with Materials of Institute Lavoisier-100(Fe) (MIL-100(Fe)) by the layer-by-layer self-assembly method, near-infrared light-triggered UCNR@MIL-100(Fe) nanomaterials with excellent antibacterial performances were constructed. A core–shell structure was constructed and confirmed by transmission electron microscopy (TEM). Reactive oxidizing species (ROS) detection indicated that the nanomaterials owned good photodynamic efficacy. The antibacterial experiments showed that the nanomaterials with 980 nm light irradiation and hydrogen peroxide (H2O2) had good antibacterial activity against Gram-negative and Gram-positive bacteria. Under 980 nm laser excitation, UCNRs generated ultraviolet and visible light to activate MIL-100(Fe) and induced a photo-Fenton reaction, which further produced oxygen species for antibacterial applications.

研究领域: 纳米技术 · 材料科学 · 生物医学工程 · 化学 · 微生物学
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Theranostics · 2013 · IF 7.806

Upconversion Nanophosphors Naluf4:Yb,Tm for Lymphatic Imaging In Vivo by Real-Time Upconversion Luminescence Imaging under Ambient Light and High-Resolution X-ray CT

Yun Sun,Juanjuan Peng,Wei Feng,Fuyou Li

Lanthanide upconversion nanophosphor (UCNP) has attracted increasing attention for potential applications in bioimaging due to its excellence in deep and high contrast imaging. To date, most upconversion imaging applications were demonstrated in dark surroundings without ambient light for higher signal-to-noise ratio, which hindered the application of optical imaging guided surgery. Herein, the new established NaLuF 4 -based UCNP (NaLuF 4 :Yb,Tm, ~17 nm) with bright upconversion emission around 800 nm as imaging signal was used to realize imaging under ambient light to provide more convenient for clinician. Moreover, due to the existance of heavy element lutetium (Lu) in the host lattice, the NaLuF 4 :Yb,Tm nanoparticles can also be used as an X-ray CT imaging agent to enhance the imaging depth and in vivo imaging resolution.

研究领域: 生物医学工程 · 纳米医学 · 医学影像学
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ACS Applied Nano Materials · 2022 · IF 6.14

Ti3C2 MXene Nanosheets Functionalized with NaErF4:0.5%Tm@NaLuF4 Nanoparticles for Dual-Modal Near-Infrared IIb/Magnetic Resonance Imaging-Guided Tumor Hyperthermia

Jialin Pan,Meiling Zhang,Gege Fu,Li Zhang,Huimei Yu,Xu Yan,Fangmeng Liu,Peng Sun,Xiaoteng Jia,Xiaomin Liu,Geyu Lu

Although the advent of two-dimensional (2D) MXenes has substantially increased the family of 2D materials and diverse applications, the rational design of MXene-based composites and their specialized applications in theranostic biomedicine remain a challenge. In this work, we developed, for the first time, Ti3C2 MXene nanosheets for near-infrared (NIR)-IIb (1530 nm) and magnetic resonance (MR) imaging-guided photothermal therapy. Surface engineering and functionalization of 2D Ti3C2 MXene nanosheets with NaErF4:0.5%Tm@NaLuF4 (NaErF4) nanoparticles result in NaErF4@Ti3C2 composites that emit in the NIR-IIb region at 1530 nm under 808 nm excitation, conferring NIR-IIb imaging guidance and monitoring capabilities during tumor hyperthermia. Due to the inherent magnetic properties of the Er3+ ions, the NaErF4@Ti3C2 composite can also be used for efficient T2-weighted MR imaging. In particular, based on the high photothermal conversion capability (43.62% at 808 nm irradiation) and photothermal stability, the designed composites were further explored for efficient tumor ablation with an inhibition ratio of 92.9%, which was systematically demonstrated both in vitro and in vivo. No significant nanocomposite toxicity was observed at the injected dose. This work not only expands the performance of MXene-based multifunctional nanostructures but also highlights the promise of their versatile applications in cancer therapy.

研究领域: 材料科学 · 生物医学工程 · 纳米医学 · 癌症治疗
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Materials Express · 2023 ·Vol. 13 ·期 11 ·1915-1921 · IF 0.7

DNAzyme modified NaYF4: Yb, Tm, Gd for near-infrared fluorescence detection of uranyl

Chen Sihan,Hu Huiqi,Jiang Wenting,Zhang Yuyun,Luo Xiaohu,Peng Jiayi,Li Le,Zhen Deshuai,Wang Hanqing

A novel near-infrared induced upconversion sensor for the detection of uranyl ions was successfully constructed using β-NaYF4: Yb, Tm, Gd upconversion nanoparticles (UCNPs) and specific DNAzyme. Characterization of the UCNPs@DNAzyme was conducted using XRD, TEM, FT-IR and fluorescence testing, and it was shown that the β-NaYF4: Yb, Tm, Gd nanoparticles were successfully prepared (∼27 nm). Upon 980 nm excitation, the UCNPs@DNAzyme emitted green light at λ=475 nm. Furthermore, Förster resonance energy transfer was observed between the UCNPs@DNAzyme (doner) and uranyl (acceptor) present on the substrate chain. This resulted in fluorescence quenching, which was used to quantify the concentration of uranyl. The developed method was found to be highly selective and sensitive, with a detection limit as low as 43 nM. This method also demonstrated excellent specificity and sensitivity for the determination of uranyl in water samples, indicating its potential application in near-infrared fluorescence detection and imaging of uranyl in vivo.

研究领域: 分析化学 · 材料科学 · 环境科学 · 纳米技术
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RSC Advances · 2017 ·Vol. 7 ·期 60 ·37929-37937 · IF 3.108

Core@shell Fe3O4@Mn2+-doped NaYF4:Yb/Tm nanoparticles for triple-modality T1/T2-weighted MRI and NIR-to-NIR upconversion luminescence imaging agents

Yang Luo,Sinan Du,Wei Zhang,Zhengfang Liao,Fang Zuo,Shengtao Yang

Core@shell structures of Fe3O4@Mn2+-doped NaYF4:Yb/Tm nanoparticles (NPs) with multifunctional properties were prepared using a hydrothermal route with a seed-growth procedure. The effect of Mn2+ ions on the phase, shape, and upconversion luminescence (UCL) of Fe3O4@Mn2+-doped NaYF4:Yb/Tm NPs was explored using X-ray diffraction, transmission electron microscopy, dynamic light scattering, and photoluminescence spectroscopy. Furthermore, hydrophobic to hydrophilic surface modification of the Fe3O4@Mn2+-doped NaYF4:Yb/Tm NPs was achieved by coating the NPs with an amphiphilic polymer (poly(maleic anhydride-alt-1-octadecene) (C18PMH)) modified with amine-functionalized methyl ether poly(ethylene glycol). Then, the NIR-to-NIR UCL ascribed to the Tm3+ ions, T1-weighted MRI ascribed to the Mn2+ ions, and T2-weighted MRI ascribed to the Fe3O4 core of the hydrophilic Fe3O4@Mn2+-doped NaYF4:Yb/Tm NPs were evaluated. The results indicate that Mn2+ doping is an effective method to control the size/shape and improve the UCL intensity of Fe3O4@Mn2+-doped NaYF4:Yb/Tm NPs, which are promising as imaging agents for NIR-to-NIR UCL and T1/T2-weighted MRI in biomedical research.

研究领域: 生物医学工程 · 材料科学 · 影像医学
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2017 ·Vol. 409 ·期 10 ·2675-2683 · IF 3.431

Near-infrared-emitting NaYF4:Yb,Tm/Mn upconverting nanoparticle/gold nanorod electrochemiluminescence resonance energy transfer system for sensitive prostate-specific antigen detection

Gao Ni,Ling Bo,Gao Zhongling,Wang Lun,Chen Hongqi

An electrochemiluminescence resonance energy transfer (ECL-RET) system that detects prostate-specific antigen (PSA) was created. Near-infrared (NIR)-emitting NaYF 4 :Yb,Tm/Mn upconverting nanoparticles (UCNPs) are used as donors, and gold nanorods (GNRs) are used as acceptors. The ECL was enhanced nearly threefold by Mn 2+ doping, with an emission peak appearing at an NIR wavelength of 808 nm. Anti-PSA 1 (Ab 1 ) was bound to the surfaces of UCNPs after being modified with poly(acrylic acid) (PAA). As for acceptors, cetyltrimethylammonium bromide (CTAB)-capped GNRs were treated with 11-mercaptoundecanoic acid (MUDA) and then conjugated with Anti-PSA 2 (Ab 2 ). When PSA was added, donors and acceptors were brought in close proximity through specific interactions of antibodies and antigens, resulting in high quenching efficiency levels. Under optimal conditions, the linear range of detection was 3.75–938 pg/mL for PSA ( R  = 0.999), with a detection limit as low as 3.16 pg/mL. This method can be applied to detect PSA in human serums with satisfactory results. An electrochemiluminescence resonance energy transfer system was developed for determination of prostate-specific antigen using near-infrared-emitting NaYF 4 :Yb,Tm/Mn upconverting nanoparticles as donors and gold nanorods as acceptors.

研究领域: 分析化学 · 纳米技术 · 生物传感器 · 癌症诊断
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2016 · IF 2.653

Aptamer biosensor for Salmonella typhimurium detection based on luminescence energy transfer from Mn2 +-doped NaYF4:Yb, Tm upconverting nanoparticles to gold nanorods

Keyi Cheng,Jianguo Zhang,Liping Zhang,Lun Wang,Hongqi Chen

A highly sensitive luminescent bioassay for the detection of Salmonella typhimurium was fabricated using Mn 2   + -doped NaYF 4 :Yb,Tm upconversion nanoparticles (UCNPs) as the donor and gold nanorods (Au NRs) as the acceptor and utilizing an energy transfer (LET) system. Mn 2   + -doped NaYF 4 :Yb,Tm UCNPs with a strong emission peak at 807   nm were obtained by changing the doped ion ratio. Carboxyl-terminated Mn 2   + -doped NaYF 4 :Yb,Tm UCNPs were coupled with S. typhimurium aptamers, which were employed to capture and concentrate S. typhimurium . The electrostatic interactions shorten the distance between the negatively charged donor and the positively charged acceptor, which results in luminescence quenching . The added S. typhimurium leads to the restoration of luminescence due to the formation of UCNPs-aptamers- S. typhimurium , which repels the UCNPs-aptamers from the Au NRs. The LET system does not occur because of the nonexistence of the luminescence emission band of Mn 2   + -doped NaYF 4 :Yb,Tm UCNPs, which had large spectral overlap with the absorption band of Au NRs. Under optimal conditions, the linear range of detecting S. typhimurium was 12 to 5   ×   10 5   cfu/mL (R   =   0.99). The limit of detection for S. typhimurium was as low as 11   cfu/mL in an aqueous buffer. The measurement of S. typhimurium in milk samples was satisfied in accordance with the plate-counting method, suggesting that the proposed method was of practical value in the application of food security.

研究领域: 生物传感器 · 微生物学 · 纳米技术 · 食品安全
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TALANTA · 2017 · IF 4.162

A near-infrared luminescent Mn2+-doped NaYF4:Yb,Tm/Fe3+ upconversion nanoparticles redox reaction system for the detection of GSH/Cys/AA

Liping Zhang,Bo Ling,Lun Wang,Hongqi Chen

An upconversion luminescence method was developed for the determination of glutathione (GSH), L -cysteine (Cys) or L -ascorbic acid (AA) based on redox reaction . We synthesized poly(acrylic acid) (PAA)-modified Mn 2+ -doped NaYF 4 :Yb,Tm upconversion nanoparticles (UCNPs), and the luminescence of these UCNPs was effectively quenched due to their carboxyl groups coordinating with Fe 3+ to form a UCNPs/Fe 3+ system. GSH, Cys or AA reduced Fe 3+ to Fe 2+ , which induced the luminescence recovery of the UCNPs. Under the optimized conditions, wide linear concentration ranges from 0.25-300   μM for GSH, 0.5–875   μM for Cys and 0.5–350   μM for AA were found, and the detection limits (3   S/K) were 0.2   μM, 0.5   μM and 0.2   μM, respectively. Thus, the UCNPs/Fe 3+ system was successfully applied for sensing GSH, Cys or AA.

研究领域: 纳米技术 · 分析化学 · 生物化学
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