研究目的
Investigating the synthesis, characterization, electrochemical properties, and fluorescence modulation interactions with carbon dots of heterobimetallic Fe(II)/Pt(II) supramolecular coordination complexes using 1,1'-ferrocene dicarboxylate and Pt(II) acceptor clips with different binding angles.
研究成果
The research successfully synthesized and characterized new heterobimetallic SCCs, demonstrating their electrochemical activity and unique interactions with carbon dots. The angular disposition of Pt(II) clips influences fluorescence quenching, with macrocycles mitigating quenching effects. This paves the way for using such systems in sensing and material applications, with potential for future host-guest and biological studies.
研究不足
The study is limited to specific Pt(II) clips and ferrocene donor; generalizability to other metals or ligands is not established. X-ray crystals of macrocycles were not obtained, relying on molecular modeling. The fluorescence modulation effects may vary with different CD syntheses or concentrations. Biological applications were not explored.
1：Experimental Design and Method Selection:
The study involved the synthesis of a new Pt(II)-based ditopic acceptor clip (3) and its use, along with two existing clips (1 and 2), in self-assembly reactions with 1,1'-ferrocenedicarboxylate to form heterobimetallic SCCs. Coordination-driven self-assembly was employed, leveraging the flexibility of the ferrocene ligand and the predefined geometry of Pt(II) clips.
2：Sample Selection and Data Sources:
Starting materials included 2,5-dibromopyrazine, trimethylsilane acetylene, trans-PtI2(PEt3)2, silver nitrate, and disodium ferrocenedicarboxylate, all commercially sourced. Carbon dots were synthesized from citric acid and cysteamine via hydrothermal method.
3：List of Experimental Equipment and Materials:
Equipment included Schlenk flasks, rotary evaporator, column chromatography setup, melting point apparatus (SRS EZ-Melt), FTIR spectrophotometer (PerkinElmer Spectrum 400), NMR spectrometer (Bruker 400 MHz), mass spectrometer (Bruker Impact ESI-Q-TOF), UV-vis spectrophotometer (Shimadzu UV-2550), spectrofluorometer (Horiba Jobin Yvon Fluoromax-4P), and time-resolved fluorescence spectrophotometer (Edinburgh Instruments LifeSpec-II). Materials were solvents like toluene, dichloromethane, acetone, and reagents as listed.
4：Experimental Procedures and Operational Workflow:
Synthesis of clip 3 involved Sonogashira cross-coupling and reaction with trans-PtI2(PEt3)
5：For SCCs (4-6), clips were treated with AgNO3 to form dinitrate derivatives, then reacted with ferrocenedicarboxylate in
1 ratio, stirred, precipitated, and purified. Characterization used NMR, MS, FTIR, and X-ray crystallography. Electrochemical studies used cyclic voltammetry. Interaction with CDs involved incubating SCCs with CD solutions and measuring UV-vis absorption and fluorescence.
6：Data Analysis Methods:
NMR and MS data were processed with standard software. Electrochemical data analyzed for E1/2 and comproportionation constants. Fluorescence data analyzed using Stern-Volmer plots and lifetime measurements.
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