properties associated with nanoclusters' molecule-like structure and energetics. Most notably, metal nanoclusters rose to research prominence in connection to the discovery of outstanding optoelectronic properties and have found practical application within catalysis, bioimaging, lighting and molecular sensing. [1][2][3][4][5][6] However, nanocluster' stabilization remains a significant impediment owing to their tendency to merge and form ever-larger aggregates at the loss of their interesting properties. Therefore, research efforts have been devoted to developing novel synthetic strategies to stabilize isolated metal nanoclusters; [7] popular approaches have often taken the form of using organic scaffolds such as DNA/RNA, proteins, and polymers. [8][9][10][11][12][13][14][15][16] The use of organic molecules gives rise to high synthesis yields, good luminescence performance, and strong compatibility with living organism, making them excellent candidates as fluorophores. Unfortunately, a main drawback is their poor long-term stability, especially in solid form, hindering their application, e.g., within lighting devices. On the other hand, template-mediated strategies based on the self-organization of the metal nanocluster within a confined volume (so-called "ship-in-a-bottle" approach) provide a promising alternative, one where the size and shape of the final metal nanocluster are dictated by the spatial restrictions imposed by the rigid host nanostructure. [17] To date, common templating structures have included glass matrices, [18] metal-organic frameworks, [19] and porous aluminosilicate zeolite crystals. [20] Here, we will shine light on zeolites as a promising scaffold for the assembly of highly luminescent and functional silver nanoclusters (Ag-NCs) within their (nano)porous interior (Figure 1a-c). As a host framework, zeolites possess molecular-sized channels and cages which enable them to confine molecules or metal (oxide) clusters inside their crystalline interior in a controlled fashion. Moreover, the framework is negatively charged, requiring counter-balancing extra-framework cations, which can be easily replaced through simple exchange methods. As shown in Figure 1d, forming the caged Ag-NCs involves a scalable bottom-up approach, whereby Ag + ions are made to self-assemble into nanoclusters via energy-driven activation (thermal treatment, photoactivation, or X-rays irradiation). Once the cluster is assembled, its optical response can be further tuned by the intentional exchange of additional guest
Metal clusters confined inside zeolite materials display remarkable luminescent properties, making them very suitable as potential alternative phosphors in white LED applications. However, up to date, only single-color emitters have been reported for luminescent metal-exchanged zeolites. In this study, we synthesized and characterized white emitting silver-sulfur zeolites, which show a remarkable color tunability upon the incorporation of silver species in highly luminescent sulfur-zeolites. Via a combined steady-state and time-resolved photoluminescence spectroscopy characterization, we suggest that the observed luminescence and tunability arise from the presence of two different species. The first associated to an orange-red emitting silver cluster (Ag-CL), whereas the second is related to a blue-white emitting SAg species. The relative contribution of both luminescent species depends on the synthesis procedure. It was shown that the formation of the blue-white emitting SAg species is favored upon a heat-treatment of the samples.
The temperature- and co-cation-dependent photoluminescence of zeolite confined Ag clusters was systematically investigated. Bright polychromatic emission and intriguing excited-state dynamics were observed and a kinetic model was proposed.
Recently, the detection and quantification of humidity has attracted great interest, but for fluorescence sensing of humidity, it is still a challenge to achieve high-performance. Here, we report an ultrasensitive...
The development of improved catalysts capable of performing the Suzuki coupling reaction has attracted considerable attention. Recent findings have shown that the use of photoactive catalysts improves the performance, while the reaction mechanism and temperature-dependent performance of such systems are still under debate. Herein, we report Pd nanocubes/CsPbBr3 as an efficient catalyst for the photothermal Suzuki reaction. The photo-induced and thermal contribution to the overall catalytic performance has been investigated. Light controls the activity at temperatures around and below 30 °C, while thermal catalysis determines the reactivity at higher temperatures. The Pd/CsPbBr3 catalyst exhibits 11 times higher activity than pure CsPbBr3 at 30 °C due to reduced activation barrier and facilitated charge carrier dynamics. Furthermore, the alkoxide radicals (R–O–) for the Suzuki reaction are experimentally and theoretically confirmed, and photogenerated holes are proven to be crucial for cleaving C–B bonds of phenylboronic acids to drive the reaction. This work prescribes a general strategy to study photothermal catalysis and offers a mechanistic guideline for photothermal Suzuki reactions.
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