研究目的
To investigate the effect of systematic replacement of secondary ligands on the photoluminescence enhancement of monolayer protected silver clusters and to develop applications such as O2 sensing.
研究成果
Systematic replacement of secondary ligands, particularly with longer-chain diphosphines, significantly enhances the photoluminescence of silver clusters through increased ligand-to-metal charge transfer and restricted intramolecular rotation. This leads to phosphorescent emission, enabling applications like O2 sensing. The approach is effective for both Ag29 and Ag51 clusters, offering a versatile method for property modification in nanoclusters.
研究不足
The study is limited to specific silver clusters and ligands; generalizability to other metal clusters or ligands is not established. Computational models used simplified structures, which may not fully capture solution-state dynamics. The O2 sensor is prototypical and requires further development for practical applications.
1：Experimental Design and Method Selection:
The study involved synthesizing silver clusters with different secondary ligands (monophosphines and diphosphines) to observe PL enhancement. Computational modeling using DFT and TDDFT was employed to understand structural and electronic changes.
2：Sample Selection and Data Sources:
Silver clusters [Ag29(BDT)12(X)4]3? and [Ag51(BDT)19(X)3]3? were synthesized, where X includes PPh3, DPPM, DPPE, DPPP, TTP, TFPP, TCPP. Samples were characterized using UV-vis spectroscopy, ESI MS, NMR, XPS, DLS, and time-resolved spectroscopy.
3：List of Experimental Equipment and Materials:
Chemicals like BDT, NaBH4, phosphines from Sigma-Aldrich and Rankem; solvents like DCM, DMF, MeOH; instruments include PerkinElmer Lambda 25 spectrometer, Waters Synapt G2-Si mass spectrometer, HORIBA JOBIN YVON Nano Log, Malvern Zetasizer Nano ZSP, Omicron ESCA Probe spectrometer, Bruker 500 MHz NMR, Edinburgh Instruments LifeSpec-ps spectrophotometer.
4：Experimental Procedures and Operational Workflow:
Clusters were synthesized via reported methods and ligand exchange. Characterization involved optical absorption, mass spectrometry, NMR, XPS, DLS, and PL measurements. O2 sensing was tested by purging gases and measuring PL changes.
5：Data Analysis Methods:
Data were analyzed using software like F900 for lifetime fitting, and computational methods in GPAW for DFT and TDDFT calculations. Quantum yields were calculated using standard equations.
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