Long-lived luminescent metal-organic frameworks (MOFs) have attracted much attention due to their structural tunability and potential applications in sensing, biological imaging, security systems, and logical gates. Currently, the long-lived luminescence emission of such inorganic-organic hybrids is dominantly confined to short-wavelength regions. The long-wavelength long-lived luminescence emission, however, has been rarely reported for MOFs. In this work, a series of structurally stable long-wavelength long-lived luminescent MOFs have been successfully synthesized by encapsulating different dyes into the green phosphorescent MOFs Cd(m-BDC)(BIM). The multicolor long-wavelength long-lived luminescence emissions (ranging from green to red) in dye-encapsulated MOFs are achieved by the MOF-to-dye phosphorescence energy transfer. Furthermore, the promising optical properties of these novel long-lived luminescent MOFs allow them to be used as ink pads for advanced anticounterfeiting stamps. Therefore, this work not only offers a facile way to develop new types of multicolor long-lived luminescent materials but also provides a reference for the development of advanced long-lived luminescent anticounterfeiting materials.
Electrochemical H2O2 production through the 2‐electron oxygen reduction reaction (ORR) is a promising alternative to the energy‐intensive anthraquinone process. Herein, by simultaneously regulating the coordination number of the atomically dispersed cobalt sites and the nearby oxygen functional groups via a one‐step microwave thermal shock, a highly selective and active CoNC electrocatalyst for H2O2 electrosynthesis that exhibits a high H2O2 selectivity (91.3%), outstanding mass activity (44.4 A g−1 at 0.65 V), and large kinetic current density (11.3 mA cm−2 at 0.65 V) in 0.1 m KOH is obtained. In strong contrast to the typical CoN4 moieties for the 4‐electron ORR, the present CoNC catalyst possesses a low‐coordinated CoN2 configuration and abundant epoxide groups, which work in synergy for promoting the 2‐electron ORR, as demonstrated by a series of control experiments and theoretical simulations. This study may provide an effective avenue to modulating the composition and structure of electrocatalysts at the atomic scale, leading to the development of new electrocatalysts with unprecedented reactivity.
Rationally
designing efficient and robust catalysts for the oxygen
evolution reaction (OER) is increasingly vital for energy conversion
technologies. Herein, we develop a core–shell electrocatalyst
consisting of an amorphous/crystalline heterophase NiFe alloy encapsulated
by ultrathin graphene layers (a/c-NiFe-G) via a rapid microwave thermal
shock strategy. The amorphous/crystalline heterostructure generates
enriched active sites with high intrinsic activity, while the graphene
coatings serve as electron transport pathways and protective layers,
resulting in dramatically enhanced OER performance in 1 M KOH with
an overpotential (η10) of 250 mV at 10 mA cm–2, a Tafel slope of 36.5 mV dec–1, a high turnover frequency (TOF) of 0.87 s–1 that
is 24 times as high as that of the crystalline counterpart when evaluated
on a glassy carbon electrode. Further, when supported on porous Ni
foam, the catalyst exhibited an η10 as low as 217
mV, along with excellent durability (136 h). Various characterization
methods, including X-ray absorption fine structure analysis and density
functional theory calculations, reveal that unsaturated coordination
configurations and abundant amorphous/crystalline boundaries in a/c-NiFe-G
are responsible for its superior OER performance. This work offers
insights for constructing metastable amorphous/crystalline heterophase
catalysts toward highly efficient electrocatalysis.
Luminescent metal-organic frameworks (MOFs) (typically dye-encapsulated MOFs) are considered as one kind of interesting downconversion materials for white-light-emitting diodes (LEDs), but their quantum efficiency (QE) is not sufficient and thus needs to be significantly enhanced for practical applications. In this study, we successfully synthesized a series of Rh@bio-MOF-1 (Rh = rhodamine) with an internal QE as high as ∼79% via a solvothermal reaction followed by cation exchanges. The high efficiency of the Rh@bio-MOF-1 composites was attributable to the high intrinsic luminescent efficiency of the selected Rh dyes, the confinement effect in the bio-MOF-1 host, and the uniform particle morphology. The emission maximum could be continuously tuned from 550 to 610 nm by controlling the species and concentration of encapsulated dye molecules, showing great color tunability of the dye-encapsulated MOFs. The emission lifetime of ∼7 ns was 1 or 2 magnitude orders shorter than that of Ce- or Eu-doped inorganic phosphors, allowing for visible light communication (VLC). White LEDs, fabricated by using the synthesized Rh@bio-MOF-1 composite and inorganic phosphors of green (Ba,Sr)SiO:Eu and red CaAlSiN:Eu, exhibited a high color rendering index of 80-94, a luminous efficacy of 94-156 lm/W, and an excellent stability in color point against drive current. The Rh@bio-MOF-1 composites with tunable colors, short emission lifetime, and high QE are expected to be used for smart white LEDs with multifunctions of both lighting and VLC.
The spatial second-order interference of two independent pseudothermal light beams in a Hong-Ou-Mandel interferometer is studied experimentally and theoretically. The similar cosine modulation in the second-order coherence function as the one with entangled-photon pairs in a Hong-Ou-Mandel interferometer is observed. Two-photon interference based on Feynman's path integral theory is employed to interpret the results. The experimental results and theoretical simulations agree with each other very well.
Differences in volatile composition and descriptive flavour attributes between the dark and milk chocolate were observed. The relationship between aroma-active compounds and sensory perception in the chocolate was verified.
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