Faujasite zeolites with a regular micropore and mesopore structure have been considered desirable scaffolds to stabilize luminescent silver nanoclusters (Ag CLs), while turning of the emission properties of the confined Ag CLs is still under investigation. In this study, the desilicated and dealuminated faujasite zeolites were first prepared to modify the zeolite framework and Si/Al ratio before Ag+ loading. With thermal treatment on the thereafter Ag+-exchanged zeolites, the Ag CLs formatted inside the D6r cages showed red-shifted emission in the desilicated zeolites and blue-shifted emission in the dealuminated zeolites, so that a tunable emission in the wavelength range of 482–528 nm could be obtained. Meanwhile, the full width at half maximum of the emission spectra is also closely related with framework modification, which monotonously increases with enhancing Si/Al ratio of host zeolite. The XRD, XPS, and spectral measurements indicated that the tunable luminescence properties of Ag CLs result from the controlling of local crystal field and coupling between host lattice and luminescent center. This paper proposes an effective strategy to manipulate the emission properties of Ag CLs confined inside zeolites and may benefit the applications of noble metal clusters activated phosphors in imaging and tunable emission.
In
this research, highly luminescent silver nanoclusters (Ag NCs)
were prepared by using Na-FAUY zeolite as a scaffold to hinder their
aggregation, and efficient energy transfer from Ag NCs to Tb3+ was realized in Ag+-Tb3+ dual-exchanged Na-FAUY
zeolites and then proved by steady spectral and luminescence lifetime
measurements. Furthermore, the effects of Ag+ loading amount,
thermal treatment, and Tb3+ loading on the luminescence
properties of Ag NCs were studied, and the optimized doping and preparing
conditions were obtained. X-ray photoelectron spectroscopy together
with spectral measurements indicated that the available sites for
Tb3+ and Ag+ are competitive and Tb3+ doping may hinder the effective formation of Ag NCs. It is also
indicated that the loading of Tb3+ may lead to reduced
Si/Al ratios, which greatly influence the luminescence property and
chemical state of Ag NCs, e.g., a high Si/Al ratio leads to blueshift
emission and stronger ionic of Ag NCs. This research may benefit
the design of Ag NCs-involved luminescent zeolites that have potential
applications for photonic devices like LEDs and 3D displays.
Silver
nanoclusters (Ag NCs) are emissive centers that are characteristic
of high quantum yield, tunable emission, and large Stokes shift when
confined inside zeolites, and their luminescence property is closely
related to the cluster size, charge state, local environment, and
extra activation. In this research, we evaluated the luminescence
response of Ag NCs on the extra-framework cations by considering Na-type
FAU-Y (NaY) as the parent zeolite. The extra-framework cations Na+ were partially substituted with Li+ or Ca2+ through the ion-exchange method and analyzed by X-ray diffraction
(XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform
infrared (FT-IR) measurements, based on which a series of MYAg (M
= Na, Li, Ca) zeolites were prepared through subsequent Ag+ exchange and thermal treatment under 600 °C for 2 h. The influence
of extra-framework cations on the lattice parameter of the host zeolite,
the exchange efficiency of Ag+, the formation ability,
and the chemical state and luminescence property of Ag NCs was studied
through the combination of structural and spectral measurements. This
research indicated a flexible pathway for manipulating the luminescence
property of Ag NCs, and the extra-framework cation-dependent luminescence
property enables the FAU-Y zeolite to become a desirable host for
the stabilization of Ag NCs to achieve highly efficient tunable emission.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.