研究目的
To design and fabricate a fluorescence probe by integrating lanthanide ions with metal-organic frameworks (MOFs) for the intelligent sensing of homovanillic acid (HVA), a biomarker of tumors and Parkinson's disease, and to integrate the sensing system with a logic gate for enhanced detection capabilities.
研究成果
The developed luminescence-based sensor integrated with a logic gate successfully detected HVA with high sensitivity and selectivity, demonstrating potential for early diagnosis of tumors. The ratiometric approach and logic gate integration enhance reliability and intelligence in sensing, paving the way for future applications in real-time clinical diagnostics.
研究不足
The study primarily focused on in vitro testing with simulated serum conditions; real-time application in human biological samples may require further validation. The probe's performance in complex biological matrices with potential interferents beyond those tested was not extensively explored. Optimization for clinical use, such as stability in varying physiological conditions, was not fully addressed.
1:Experimental Design and Method Selection:
The study involved designing a lanthanide MOF (LMOF) with dual-emission centers for ratiometric sensing of HVA. The probe was synthesized under hydrothermal conditions, and its sensing capabilities were evaluated through fluorescence spectroscopy. A logic gate operation was integrated to process the fluorescence signals for intelligent sensing.
2:Sample Selection and Data Sources:
HVA and other serum constituents (e.g., glucose, creatinine, NaCl) were used as analytes. Goat serum was pretreated with acetonitrile to remove proteins for real-sample testing.
3:List of Experimental Equipment and Materials:
Equipment included Bruker D8 diffractometer (XRD), Tensor 27 FTIR spectrometer, Cary 60 UV-vis spectrophotometer, FLS920 photoluminescence spectrometer, X-7 series ICP-MS, Netzsch STA 449C TGA system, and RBD upgraded PHI-5000C ESCA system (XPS). Materials included 1,2,4,5-benzenetetracarboxylic acid (H4btec), Al(NO3)3·9H2O, Tb(NO3)3·6H2O, and various chemicals for interference studies.
4:Experimental Procedures and Operational Workflow:
Synthesis of Al(OH)[H2btec] (1) via hydrothermal reaction at 210°C for 24 h, followed by activation. Preparation of Tb3+@1 by stirring compound 1 with Tb(NO3)3·6H2O in ethanol. Characterization using XRD, FTIR, UV-vis, PL, ICP-MS, TGA, and XPS. Sensing experiments involved immersing Tb3+@1 in HVA solutions and measuring fluorescence intensities at 340 nm and 544 nm. Logic gate implementation used normalized intensity values with a threshold of 0.
5:Data Analysis Methods:
5. 5. Data Analysis Methods: Fluorescence intensity ratios (I340 nm/I544 nm) were plotted against HVA concentrations for sensitivity analysis. Limit of detection (LOD) was calculated using the 3σ IUPAC criteria. Statistical analysis included linear regression (R2 = 0.945) and reproducibility checks with triplicate experiments.
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Diffractometer
D8
Bruker
Powder X-ray diffraction (XRD) data collection for structural analysis of synthesized materials.
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FTIR Spectrometer
Tensor 27
Bruker
Fourier transform-infrared (FTIR) spectra acquisition to analyze chemical bonds and functional groups.
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UV-Vis Spectrophotometer
Cary 60
Agilent
Ultraviolet-visible (UV-vis) absorption spectra measurement for optical properties analysis.
Cary 60 UV-Vis Spectrophotometer
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Photoluminescence Spectrometer
FLS920
Perkin-Elmer Edinburgh
Photoluminescence (PL) spectra and emission lifetimes recording for fluorescence characterization.
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ICP-MS
X-7 series
Thermo Elemental
Inductively coupled plasma-mass spectrometry for elemental analysis, specifically Tb3+ and Al3+ measurement.
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XPS System
RBD upgraded PHI-5000C ESCA
PerkinElmer
X-ray photoelectron spectroscopy for surface chemical analysis and confirmation of Tb3+ loading.
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TGA System
Netzsch STA 449C
Netzsch
Thermogravimetric analysis to assess thermal stability and decomposition of materials.
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