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Emerging switchable ultraviolet photoluminescence in dehydrated Zn/Al layered double hydroxide nanoplatelets.

ABSTRACT: Layered double hydroxides show intriguing physical and chemical properties arising by their intrinsic self-assembled stacking of molecular-thick 2D nanosheets, enhanced active surface area, hosting of guest species by intercalation and anion exchanging capabilities. Here, we report on the unprecedented emerging intense ultraviolet photoluminescence in Zn/Al layered double hydroxide high-aspect-ratio nanoplatelets, which we discovered to be fully activated by drying under vacuum condition and thermal desorption as well. Photoluminescence and its quenching were reproducibly switched by a dehydration-hydration process. Photoluminescence properties were comprehensively evaluated, such as temperature dependence of photoluminescence features and lifetime measurements. The role of 2D morphology and arrangement of hydroxide layers was demonstrated by evaluating the photoluminescence before and after exfoliation of a bulk phase synthetized by a coprecipitation method.

SUBMITTER: Prestopino G

PROVIDER: S-EPMC6687718 | biostudies-literature | 2019 Aug

REPOSITORIES: biostudies-literature

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Emerging switchable ultraviolet photoluminescence in dehydrated Zn/Al layered double hydroxide nanoplatelets.

Prestopino G G Arrabito G G Generosi A A Mattoccia A A Paci B B Perez G G Verona-Rinati G G Medaglia P G PG

Scientific reports 20190808 1

Layered double hydroxides show intriguing physical and chemical properties arising by their intrinsic self-assembled stacking of molecular-thick 2D nanosheets, enhanced active surface area, hosting of guest species by intercalation and anion exchanging capabilities. Here, we report on the unprecedented emerging intense ultraviolet photoluminescence in Zn/Al layered double hydroxide high-aspect-ratio nanoplatelets, which we discovered to be fully activated by drying under vacuum condition and the ...[more]

PMID: 31395962

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Project description:Layered double hydroxides (LDHs) are an ideal platform to host catalytic metal centers for water oxidation (WO) owing to the high accessibility of water to the interlayer region, which makes all centers potentially reachable and activated. Herein, we report the syntheses of three iridium-doped zinc-aluminum LDHs (Ir-LDHs) nanomaterials (1-3, with about 80 nm of planar size and a thickness of 8 nm as derived by field emission scanning electron microscopy and powder X-ray diffraction studies, respectively), carried out in the confined aqueous environment of reverse micelles, through a very simple and versatile procedure. These materials exhibit excellent catalytic performances in WO driven by NaIO4 at neutral pH and 25 °C, with an iridium content as low as 0.5 mol % (∼0.8 wt %), leading to quantitative oxygen yields (based on utilized NaIO4, turnover number up to ∼10,000). Nanomaterials 1-3 display the highest ever reported turnover frequency values (up to 402 min-1) for any heterogeneous and heterogenized catalyst, comparable only to those of the most efficient molecular iridium catalysts, tested under similar reaction conditions. The boost in activity can be traced to the increased surface area and pore volume (>5 times and 1 order of magnitude, respectively, higher than those of micrometric materials of size 0.3-1 μm) estimated for the nanosized particles, which guarantee higher noble metal accessibility. X-ray absorption spectroscopy (XAS) studies suggest that 1-3 nanomaterials, as-prepared and after catalysis, contain a mixture of isolated, single octahedral Ir(III) sites, with no evidence of Ir-Ir scattering from second-nearest neighbors, excluding the presence of IrO2 nanoparticles. The combination of the results obtained from XAS, elemental analysis, and ionic chromatography strongly suggests that iridium is embedded in the brucite-like structure of LDHs, having four hydroxyls and two chlorides as first neighbors. These results demonstrate that nanometric LDHs can be successfully exploited to engineer efficient WOCs, minimizing the amount of iridium used, consistent with the principle of the noble-metal atom economy.

Dataset Information

Emerging switchable ultraviolet photoluminescence in dehydrated Zn/Al layered double hydroxide nanoplatelets.

Publications

Emerging switchable ultraviolet photoluminescence in dehydrated Zn/Al layered double hydroxide nanoplatelets.

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