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LANGMUIR · 2014 · IF 4.384

Turn-On Detection of a Cancer Marker Based on Near-Infrared Luminescence Energy Transfer from NaYF4:Yb,Tm/NaGdF4 Core–Shell Upconverting Nanoparticles to Gold Nanorods

Hongqi Chen,Yingying Guan,Shaozhen Wang,Yuan Ji,Mengqi Gong,Lun Wang

A homogeneous immunoassay for the sensitive and selective determination of trace amounts of α-fetoprotein (AFP, a cancer marker) by detection in the near-infrared (NIR) region based on luminescence energy transfer (LET) from NaYF4:Yb,Tm/NaGdF4 core–shell upconverting nanoparticles to gold nanorods (GNRs) is presented. The carboxyl-functionalized NaYF4:Yb,Tm/NaGdF4 core–shell upconverting nanoparticles (UCNPs) were excited by a 980 nm continuous wavelength laser, and its emission peak appeared at a near-infrared wavelength (∼804 nm). The carboxyl-functionalized upconverting nanoparticles were conjugated with the anti-AFP (Ab1) and acted as donor. GNRs with a high absorption band around 790 nm, which was overlapped the UCNPs emission, were synthesized and acted as the acceptor. The donor (negatively charged) interacted with the acceptor (positively charged) via electrostatic interactions to bring them into close proximity. LET could occur, producing a quenching phenomenon. When the AFP antigens were added into the system, the binding affinity between AFP and Ab1 was stronger than the electrostatic interactions, which released the energy acceptors from the energy donors, interrupting luminescence energy transfer, and therefore, the luminescence was recovered. On the basis of the restored luminescence, a turn-on optical immunosening system was developed. Under the optimal conditions, the linear range of detection was from 0.18 to 11.44 ng/mL for AFP (R = 0.99), with a detection limit as low as 0.16 ng/mL. The proposed method has also been used to monitor AFP in human serum samples. Therefore, further study based on the NaYF4:Yb,Tm/NaGdF4 core–shell nanoparticles-GNRs construction may open the way for a new class of NIR-LET biosensors with wide applications.

研究领域: 生物医学工程 · 分析化学
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Nanophotonics · 2020 ·Vol. 9 ·期 6 ·1519-1528 · IF 7.491

Pumping-controlled multicolor modulation of upconversion emission for dual-mode dynamic anti-counterfeiting

Xiaoru Dai,Ke Wang,Lei Lei,Shiqing Xu,Yao Cheng,Yuansheng Wang

Lanthanide up-conversion features stepwise multi-photon processes, where the difference in photon number that is required for specific up-conversion process usually leads to significant variance in pumping-related processes/properties. In this work, a pumping-controlled dual-mode anti-counterfeiting strategy is conceived by taking advantage of the combination of up-conversion processes with different photon numbers. The combination of Er 3+ and Tm 3+ , which are spatially separated within a designed core/triple-shell nano-architecture, is taken as an example to illustrate such idea. Upon infrared excitation, the emission color of a designed pattern can be switched from red to purple by increasing the excitation power density from 5 to 11 W/cm 2 , while a bright luminescent trajectory including red, white and blue-green color with different length is observed when rotating the pattern above 600 rpm. In addition, the relative up-conversion emission intensities of the Er 3+ and Tm 3+ ions can be manipulated through tailoring interfacial or inner defects in the core/triple-shell nano-crystals, which enable an ultrahigh sensitivity for the pumping-controlled emission color variation to be observed under excitation power well below 11 W/cm 2 .

研究领域: 材料科学 · 纳米技术 · 光学 · 光子学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-10 · IF 16.6

Ultra-wideband-responsive photon conversion through co-sensitization in lanthanide nanocrystals

Jiang Zhao,He Liangrui,Yang Zhiwen,Qiu Huibin,Chen Xiaoyuan,Yu Xujiang,Li Wanwan

Distinctive upconversion or downshifting of lanthanide nanocrystals holds promise for biomedical and photonic applications. However, either process requires high-energy lasers at discrete wavelengths for excitation. Here we demonstrate that co-sensitization can break this limitation with ultrawide excitation bands. We achieve co-sensitization by employing Nd 3+ and Ho 3+ as the co-sensitizers with complementary absorptions from the ultraviolet to infrared region. Symmetric penta-layer core-shell nanostructure enables tunable fluorescence in the visible and the second near-infrared window when incorporating different activators (Er 3+ , Ho 3+ , Pr 3+ , and Tm 3+ ). Transient spectra confirm the directional energy transfer from sensitizers to activators through the bridge of Yb 3+ . We validate the features of the nanocrystals for low-powered white light-emitting diode-mediated whole-body angiography of mice with a signal-to-noise ratio of 12.3 and excitation-regulated encryption. This co-sensitization strategy paves a new way in lanthanide nanocrystals for multidirectional photon conversion manipulation and excitation-bandwidth-regulated fluorescence applications.

研究领域: 纳米技术 · 生物光子学 · 材料科学 · 生物医学工程
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ACS Applied Nano Materials · 2024 · IF 5.3

Dual-Mode Luminescence from Polyacrylonitrile-Stabilized CsPbX3 (X = Br and I) Nanocrystals Triggered by NaYF4:Yb/Ln (Ln = Er and Tm) Upconversion Nanoparticles: Implications for Anticounterfeiting and Optical Thermometry

Mingye Ding,Xiaoyan Wang,Yinbiao Shi,Zixia Lin,Zhengtao Deng,Xiaofei Yang

Owing to their excellent photoelectric and optical properties, lead halide perovskite quantum dots (PeQDs) have attracted great attention and have broad applications in various fields. However, the shortcomings of poor stability and short-wavelength (ultraviolet/visible) excitation restrict their practical applications. Herein, to address the above issues, we report a polyacrylonitrile-based composite film containing CsPbX3 (X = Br and I) PeQDs and β-NaYF4:Yb/Ln (Ln = Tm and Er) upconversion nanoparticles (UCNPs) via an electrospinning strategy. Interestingly, all-inorganic CsPbX3 PeQDs are synthesized through an in situ growth process in polyacrylonitrile nanofibers, which provide a polymer matrix for the protection of PeQDs against decomposition under the effect of an external environment. Upon 980 nm laser irradiation, lanthanide-sensitized UC luminescence of stable CsPbX3 can be realized through radiative energy transfer from Tm3+/Er3+ ions to PeQDs. Consequently, dual-mode luminescence, including downshifting and UC with color-tunable outputs, can be observed from PeQDs under dual-wavelength excitation (UV and NIR). Benefiting from the special luminescent feathers (temperature-sensitive UC and dual-mode luminescence), the as-obtained composite nanofibers exhibit great potential in high-level anticounterfeiting and accurate noncontact thermometry.

研究领域: 材料科学 · 纳米技术 · 光学 · 光子学
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OPTICAL MATERIALS · 2024 · IF 3.8

Multicolor luminescence and energy transfer of KSrGd(PO4)2:Ln3+ (Ln = Ce, Sm, Eu, Tb, Dy, Dy/Eu, Yb/Ho, Yb/Er, Yb/Tm) phosphors for WLED and multiple anti-counterfeiting

Mengran Ouyang,Huimin Du,Jiahao Wu,Shanshan Hu,Jun Yang

KSrGd(PO 4 ) 2 :Ln 3+ (Ln = Ce, Sm, Eu, Tb, Dy, Dy/Eu, Yb/Ho, Yb/Er, Yb/Tm) phosphors were synthesized by high temperature solid state method. Doping the KSrGd(PO 4 ) 2 matrix with 5%Dy 3+ ions resulted in white light emission under 345 nm excitation. The calculated color temperature (CCT) of this white light is 5523 K, indicating as positive white light. It was found that the luminous intensity of the obtained KSrGd(PO 4 ) 2 :5%Dy 3+ at 200 °C was 76.80 % of that at room temperature, showing good thermal stability as well as possibility of application in white LED. Under the excitation at 392 nm, the fluorescence quantum yield of KSrGd(PO 4 ) 2 :10%Eu 3+ is 79.92 %. Energy transfer between Dy 3+ and Eu 3+ is observed in KSrGd(PO 4 ) 2 :Dy 3+ /Eu 3+ samples, with identified mechanism as the quadrupole-quadrupole interaction. Tunable luminescence ranging from white to yellow then to orange-red is achieved by adjusting the doping concentration of Eu 3+ in KSrGd(PO 4 ) 2 :5%Dy 3+ , x%Eu 3+ . Under the excitation of 980 nm near-infrared light, the prepared KSrGd(PO 4 ) 2 :Yb 3+ /Ho 3+ , KSrGd(PO 4 ) 2 :Yb 3+ /Er 3+ and KSrGd(PO 4 ) 2 :Yb 3+ /Tm 3+ samples showed up-conversion emissions of red, yellow and blue, respectively, with two-photon processes. In KSrGd(PO 4 ) 2 matrix, multi-color and multi-security marks were successfully prepared by utilizing up/down conversion luminescence characteristics, which obtained good anti-counterfeiting effect and improved anti-counterfeiting security. Therefore, the obtained KSrGd(PO 4 ) 2 : Ln 3+ phosphors exhibit promising application prospects in the fields of WLED and multiple anti-counterfeiting.

研究领域: 材料科学 · 光学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Up-conversion luminescence and Bi SPR effect promoted Z-scheme BiVO4(040)-Bi-(NaYF4:Er,Yb,Tm@BiOBr)/Bi photocatalyst for efficient photocatalytic hydrogen production with simultaneous degradation of malachite green

Shuguang Li,Jize Liu,Haibo Wu,Xinxin Zhang,Yanqiong Guo,Boyang Kang,Limin Zhao

Photocatalytic hydrogen production with simultaneous degradation of organic pollutants by using solar energy provide a promising strategy to solve the energy and environmental issue in the future. However, for onefold wide band-gap semiconductor, the poor photocatalytic efficiency limits its application on a large scale due to its easy recombination of photo-generated electron-hole pairs and low solar energy utilization. Herein, a novel Z-scheme BiVO 4 (040)-Bi-(NaYF 4 :Er,Yb,Tm@BiOBr)/Bi photocatalyst is prepared via photo-assisted isoelectric point method. In this composite photocatalyst, up-convention luminescence material, NaYF 4 :Er,Yb,Tm, can offer more ultraviolet light and visible light to intensify the activations of BiOBr and metal Bi nanoparticles, respectively. Furthermore, the formation of Z-scheme BiVO 4 (040)-BiOBr photocatalystic sytem, the spatial separation of the BiVO 4 (040) and BiVO 4 (110) facets and the presence of metal Bi surface plasmon resonance effect are contributed to the high-efficiency separation of the photo-generated electron-hole pairs. The experimental results show that as-prepared Z-scheme BiVO 4 (040)-Bi-(NaYF 4 :Er,Yb,Tm@BiOBr)/Bi photocatalyst exhibits advanced photocatalytic hydrogen production amount (192.0 μm) and excellent degradation ratio of malachite green (88.51 %) under simulated sunlight irradiation for 5.0 h. The apparent quantum yield of the Z-scheme BiVO 4 (040)-Bi-(NaYF 4 :Er,Yb,Tm@BiOBr)/Bi photocatalyst at 420 nm reaches a specific value of 5.8 %. In addition, Z-scheme BiVO 4 (040)-Bi-(NaYF 4 :Er,Yb,Tm@BiOBr)/Bi photocatalyst also remains a high stability in the photocatalytic hydrogen production with simultaneous degradation of malachite green within six reuse. At last, the possible reaction mechanism and degradation pathways of malachite green caused by Z-scheme BiVO 4 (040)-Bi-(NaYF 4 :Er,Yb,Tm@BiOBr)/Bi photocatalyst under simulated sunlight irradiation are put forward.

研究领域: 材料科学 · 环境科学 · 化学工程
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Corrosion Communications · 2021 · IF 0

Preparation and molten salts corrosion behavior of high-entropy (Ca,Sr,Ba)TMO3 (TM= Zr, Hf and Ta): Promising protecting materials of reference electrode for metal smelting through fused salts electrolysis

Shuaihang Qiu,Huimin Xiang,Fu-Zhi Dai,Hailong Wang,Yanchun Zhou

The protecting materials of reference electrode with good corrosion resistance to molten salts play vital roles in realizing smelting of refractory and rare earth metals through fused salts electrolysis. BaZrO 3 has been considered as a candidate protecting material of reference electrode for its good chemical stability and high-temperature corrosion resistance. However, the unsatisfactory corrosion resistance to molten salts hinders its practical application. In order to enhance the corrosion resistance to molten salts, three perovskite structured high-entropy oxides HE (Ca,Sr,Ba) TM O 3 including (Ca,Sr,Ba)(Zr,Hf)O 3 , (Ca,Sr,Ba)(Zr,Ta)O 3 and (Ca,Sr,Ba)(Zr,Hf,Ta)O 3 , were designed and prepared in this work. The as-prepared HE (Ca,Sr,Ba)(Zr,Hf)O 3 and (Ca,Sr,Ba)(Zr,Hf,Ta)O 3 ceramics are single-phase, while the as-prepared HE (Ca,Sr,Ba)(Zr,Ta)O 3 ceramic contains 11.6 vol.% of (Ca,Sr,Ba) 2 Ta 2 O 7 . These HE (Ca,Sr,Ba) TM O 3 ceramics possess better corrosion resistance to molten NaCl-KCl salts than BaZrO 3 , among which (Ca,Sr,Ba)(Zr,Hf,Ta)O 3 shows the best corrosion resistance to molten NaCl-KCl salts. The mass loss per unite area of HE (Ca,Sr,Ba)(Zr,Hf,Ta)O 3 after corrosion by molten NaCl-KCl salts at 800 °C for 8 h is mere 2.6×10 −6  g/mm 2 which is ca . 1/60 of that of BaZrO 3 (∼1.7×10 −4  g/mm 2 ), and its surface after corrosion is plain and smooth without any new phase detectable after corrosion. It also exhibits better corrosion resistance to molten NaF-KF salts than BaZrO 3 . The mass loss per unite area after corrosion by molten NaF-KF salts at 800 °C for 8 h is only 2.9×10 −5  g/mm 2 which is smaller than that of BaZrO 3 (3.6×10 −5  g/mm 2 ), the corrosion caused by molten NaF-KF salts only occurs on the surface and the thickness of the corrosion layer is mere ∼8 µm, being less than 1/10 of that of BaZrO 3 (∼100 µm). These results indicate that the three HE (Ca,Sr,Ba) TM O 3 , especially (Ca,Sr,Ba)(Zr,Hf,Ta)O 3 , are promising as protecting materials of reference electrode for the smelting of refractory and rare earth metals through fused salts electrolysis.

研究领域: 材料科学 · 冶金工程 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Thermal properties of high-entropy fluorite (Zr0.2Hf0.2Pr0.2La0.2×0.2)O2-δ(X=Dy, Ho, Er, Y, Tm): A first-principles combined with experimental study investigating the influence of size and mass difference effect

Jiadong Hou,Yufeng Liu,Chufei Cheng,Fuhao Cheng,Pengfei Qin,Yang Miao,Weihua Ji,Xiaomin Wang

The limited efficiency of traditional trial-and-error experiments has impeded the development and application of high-entropy fluorite oxides in thermal insulation coatings. To solve this problem, a novel entropy descriptor based on first principles is presented to help select candidate components for synthesizing high-entropy fluorite structure oxides. Results show that the compatibilities of 10 single-phase high-entropy fluorite oxides can be accurately predicted based on entropy formation ability. In the studied (Zr, Hf, Pr, La, X) O 2-δ system, a correlation between thermal characteristics and size/mass differences was established by designing the size and mass of X. Specifically, we found that the thermal conductivity is more strongly correlated with the difference in atomic mass, while the coefficient of thermal expansion is strongly correlated with the difference in atomic size. X-ray photoelectron spectroscopy (XPS) analysis shows that the concentration of oxygen vacancy can effectively reduce the thermal conductivity of high-entropy fluorite oxides. In addition, the values of hardness, elastic modulus and thermal conductivity of five single-phase fluorite oxides are successfully predicted by first principles calculation , and the differences between these values and the experimental results are small, which provides a prospective significance for the performance prediction of high-entropy fluorite oxides. Our findings provide a strategy for customizing high-entropy fluorite single-phase oxides with suitable properties to meet the performance requirements of thermal barrier coatings (TBCs).

研究领域: 材料科学 · 热力学
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2024 · IF 5.7

Trehalose Ameliorates Nonalcoholic Fatty Liver Disease by Regulating IRE1α–TFEB Signaling Pathway

Shan Su,Xiaohong Liu,Min Zhu,Wen Liu,Jingyi Liu,Yujia Yuan,Fudong Fu,Zhiyong Rao,Jingping Liu,Yanrong Lu,Younan Chen

Nonalcoholic fatty liver disease (NAFLD), characterized by hepatic lipid deposition, is one of the most prevalent chronic metabolic disorders globally, and its pharmaceutical treatments are still limited. Excessive lipid accumulation triggers endoplasmic reticulum (ER) stress and autophagy flux dysfunction, which are important mechanisms for NAFLD. Trehalose (Tre), a natural disaccharide, has been identified to reduce hepatic steatosis and glucose intolerance. However, its underlying mechanisms for NAFLD remain unclear. In this study, a high-fat-diet (HFD)-induced mouse NAFLD model and a saturated fatty acid palmitic acid (PA)-stimulated cell model were constructed. The results indicated that Tre supplementation ameliorated hepatocyte lipid deposition in vitro, as well as hepatic steatosis and hyperlipidemia in vivo. Mechanistically, Tre alleviated both autophagy flux dysfunction and endoplasmic reticulum (ER) stress. Under the stimulation of HFD or PA, Tre remarkably increased the expression and nucleic translocation of the lysosomal master protein transcription factor EB (TFEB), while decreasing the accumulation of p62 and also decreasing the ER stress markers (inositol-requiring enzyme 1 (IRE1α), XBP-1, CHOP, and BIP). Similar results were observed in an ER stressor tunicamycin (TM)-induced in vivo and in vitro models. In addition, the transcriptomic analysis of NAFLD patients revealed significant differences in ER stress-related and autophagy-related biomarkers, including TFEB, ATG7, IRE1α, and CHOP. Molecular docking results demonstrated a strong affinity between Tre and both IRE1α and TFEB. Overall, Tre protected hepatocytes from lipotoxicity-related ER stress and autophagy dysfunction, and its regulatory effect on the IRE1α–TFEB signaling pathway may be a critical mechanism. These findings suggest that Tre, as a bioactive substance with significant medicinal potential, holds considerable promise for drug development and clinical application in treating NAFLD.

研究领域: 药理学 · 分子生物学 · 代谢紊乱 · 肝病学
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MICROCHIMICA ACTA · 2018 ·Vol. 185 ·期 3 ·1-9 · IF 5.705

Effect of silica surface coating on the luminescence lifetime and upconversion temperature sensing properties of semiconductor zinc oxide doped with gallium(III) and sensitized with rare earth ions Yb(III) and Tm(III)

Li Yuemei,Li Yongmei,Wang Rui,Zheng Wei

Optical sensing of temperature by measurement of the ratio of the intensities of the 700 nm emission and the 800 nm emission of Ga(III)-doped ZnO (GZO) nanoparticles (NPs) and of GZO NPs coated with a silica shell are demonstrated at 980 nm excitation. It is found that the relative sensitivity of SiO 2 @Yb/Tm/GZO is 6.2% K −1 at a temperature of 693 K. This is ~3.4 times higher than that of Yb/Tm/GZO NPs. Obviously, the SiO 2 shell structure decreases the rate of the nonradiative decay. The decay time of the 800 nm emission of the Yb/Tm/GZO NPs (15 mol% Ga; 7 mol% Yb; 0.5 mol% Tm) displays a biexponential decay with a dominant decay time of 148 μs and a second decay time of ~412 μs. The lifetime of the Yb/Tm/GZO NPs at 293 K, and of the SiO 2 @Yb/Tm/GZO NPs are ~412 μs. Both the Yb/Tm/GZO and SiO 2 @Yb/Tm/GZO can be used up to 693 K. These results indicate that the SiO 2 shell on the Yb/Tm/GZO is beneficial in terms of sensitivity and resolution. The enhancement the decay time and thermal sensitivity in the SiO 2 @Yb/Tm/GZO shell@core structure have been studied compared to the Ga(III)-doped Yb/Tm-doped ZnO (Yb/Tm/GZO). The SiO 2 @Yb/Tm/GZO have good thermal accuracy up to 693 °C.

研究领域: 光学传感 · 纳米材料 · 热力学测量 · 稀土掺杂材料 · 无机功能材料
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Chemo-Photothermal Combination Cancer Therapy with ROS Scavenging, Extracellular Matrix Depletion, and Tumor Immune Activation by Telmisartan and Diselenide-Paclitaxel Prodrug Loaded Nanoparticles

Tianxu Fang,Jun Zhang,Tiantian Zuo,Guangyu Wu,Yingxin Xu,Yifan Yang,Jie Yang,Qi Shen

Extracellular matrix (ECM) accumulating in the tumor microenvironment (TME) is generated by tumor-associated fibroblasts. It can elevate interstitial fluid pressure and form dense barriers in tumor tissues. Consequently, nanocarriers are hindered from permeating into deeper tumor sites. Thus, the programmed drug-releasing nanoparticles, G(TM)PPSP, were developed for TME remodeling and breast cancer therapy. Gelatin nanoparticles were linked with platinum nanoparticles (PtNPs) to obtain G(TM)PPSP with a size of 214.0 ± 5.0 nm. Telmisartan (TM) was loaded in gelatin nanoparticles. Paclitaxel (PTX) was attached to PtNPs via a dual redox responsive diselenide bond. TM release was mediated by MMP-2 because of gelatin degradation in TME, and then intracellular PTX was released because of diselenide linkage fracture triggered by ROS or glutathione. ECM was depleted owing to TGF-β downregulation by TM and direct ablation by the photothermal effect of PtNPs. 4T1 tumor progression was inhibited by PTX chemotherapy, intracellular ROS scavenging of PtNPs, and photothermal therapy (PTT). The tumor spheroid penetration assay proved G(TM)PPSP could permeate into deep tumor regions when MMP-2 existed. In vivo antitumor experiments implied G(TM)PPSP with PTT could inhibit tumor growth effectively and remodel TME via ECM depletion and immunity activation, indicating the potential of G(TM)PPSP-based chemo-photothermal combination therapy for breast cancer treatment.

CAS / MDL: 3326-32-7
研究领域: 癌症研究 · 纳米技术 · 药学 · 生物医学工程 · 治疗学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

NIR-Driven Water Splitting H2 Production Nanoplatform for H2-Mediated Cascade-Amplifying Synergetic Cancer Therapy

Qi Wang,Yishun Ji,Jinsheng Shi,Lili Wang

As a newly emerging treatment strategy for many diseases, hydrogen therapy has attracted a lot of attention because of its excellent biosafety. However, the high diffusivity and low solubility of hydrogen make it difficult to accumulate in local lesions. Herein, we develop a H2 self-generation nanoplatform by in situ water splitting driven by near-infrared (NIR) laser. In this work, core–shell nanoparticles (CSNPs) of NaGdF4:Yb,Tm/g-C3N4/Cu3P (UCC) nanocomposites as core encapsulated with zeolitic imidazolate framework-8 (ZIF-8) modified with folic acid as shell are designed and synthesized. Due to the acid-responsive ZIF-8 shell, enhanced permeability and retention (EPR) effect, and folate receptor-mediated endocytosis, CSNPs are selectively captured by tumor cells. Upon 980 nm laser irradiation, CSNPs exhibit a high production capacity of H2 and active oxygen species (ROS), as well as an appropriate photothermal conversion temperature. Furthermore, rising temperature increases the Fenton reaction rate of Cu(I) with H2O2 and strengthens the curative effect of chemodynamic therapy (CDT). The excess glutathione (GSH) in tumor microenvironment (TME) can deplete positive holes produced in the valence band of g-C3N4 in the g-C3N4/Cu3P Z-scheme heterojunction. GSH also can reduce Cu(II) to Cu(I), ensuring a continuous Fenton reaction. Thus, a NIR-driven H2 production nanoplatform is constructed for H2-mediated cascade-amplifying multimodal synergetic therapy.

研究领域: 纳米技术 · 癌症治疗 · 材料科学 · 光热治疗 · 化学工程 · 生物医学工程
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