Hybrid two-dimensional (2D) lead halide perovskites have been employed in optoelectronic applications, including white light emission for light emitting diodes (LEDs). However, until now, there have been limited reports on white light emitting lead halide perovskites with experimental insights into the mechanism of the broad band emission. Here, we present white light emission from a 2D hybrid lead chloride perovskite, using the widely known phenethylammonium cation. The single crystal X-ray structural data, time-resolved photophysical measurements, and DFT calculations are consistent with broad band emission arising from strong exciton-phonon coupling with the organic lattice, which is independent of surface defects. The phenethylammonium lead chloride material exhibits a remarkably high color rendering index of 84, CIE coordinate of (0.37,0.42), CCT of 4426, and photostability, making it ideal for natural white LEDs applications.
While manipulating the helicity of nanostructures is a challenging task, it attracts great research interest on account of its crucial role in better understanding the formation mechanisms of helical systems. For the supramolecular chirality in self-assembly systems, one challenge is how to understand the origin of supramolecular chirality and inherent helicity information on nanostructures regulated by functionality-oriented stacking modes (such as J- and H-aggregation) of building blocks. Herein, two-component hydrogels were prepared by phenylalanine-based enantiomers and achiral bis(pyridinyl) derivatives, where helical nanofibers with inverse handedness as well as controllable helical pitch and diameter were readily obtained through stoichiometric coassembly of these building blocks. The helix inversion was achieved by the transition between the J- and H-aggregation of bis(pyridinyl) derivatives, which was collectively confirmed by circular dichroism, scanning electron microscopy, Fourier transform infrared spectroscopy, and single X-ray crystallography. Interestingly, the helical coassemblies with opposite handedness could be obtained not only from the enantiomeric building blocks but also from the chiral monomers with the same configurational chirality by exchanging achiral additives. This work provides insight into the origin and helicity inversion of supramolecular chirality in molecular self-assembly systems and may shine light on the precise fabrication of chiral nanostructures for potential applications in smart display devices, optoelectronics, and biological systems.
Chemoselective aliphatic carbon–carbon bond activation photocatalyzed by vanadium oxo complexes under ambient conditions and visible light.
Sensory memory is capable of recording information and giving feedback based on external stimuli. Haptic memory in particular can retain the sensation of the interaction between the human body and the environment and help humans to describe the physical quantities in their environment and manipulate objects in daily activities. Although sensitive and accurate tactile sensors have been produced on optical and electronic devices, their rigorous operation and equipment requirements seriously limit their further applicability. In addition, their poor retainability after the removal of external stimuli also warrants further improvements. Thus, haptic memory materials, having simple structures and high sensitivity, are highly desired. Herein, we successfully developed two piezochromic assemblies assisted by halogen bonding for haptic memory. The halogen bond not only contributes to the fabrication of the network and enhances integrative stability but also broadens the natural piezofluorescent range, thus promoting sensory sensitivity. Moreover, the colorimetric change of the assemblies could be well-retained after the stimulus was removed. Upon mild heating treatment, the piezochromic response could be recovered to its original state, confirming the recyclability of this haptic memory material for use in practical applications. The present work enriches the library of piezochromic materials with enhanced performance for haptic memory.
Two‐dimensional lead and tin halide perovskites were prepared by intercalating the long alkyl group 1‐hexadecylammonium (HDA) between the inorganic layers. We observed visible‐light absorption, narrow‐band photoluminescence, and nanosecond photoexcited lifetimes in these perovskites. Owing to their hydrophobicity and stability even in humid air, we applied these perovskites in the decarboxylation and dehydrogenation of indoline‐2‐carboxylic acids. (HDA)2PbI4 or (HDA)2SnI4 were investigated as photoredox catalysts for these reactions, and quantitative conversion and high yields were observed with the former.
We utilized two organic dications containing, respectively, a pyridinium and an imidazolium core to construct new n = 1 (where n refers to the number of contiguous 2D inorganic layers; i.e., not separated by organic cations) twodimensional (2D) lead-iodide perovskites 1 and 2. The former material exhibits a (100)-and the latter a very rare 3 3 (110)structural type. Compared with primary ammonium functionality, their constituent ring-centred positive charges have lower charge density. As a result, [PbI6]4-inter-octahedral distortions of the inorganic lattice are reduced (Pb-I-Pb bond angles are as high as 166o and 174o, respectively). This results in bathochromically shifted optical features. In addition, the compact nature of the dications produce super short lead-iodide sheet separations, with respective iodide-iodide (I•••I) distances as small as 4.149 Å and 4.278 Å. These are amongst the shortest separations of adjacent lead-iodide layers, in such materials, ever reported. When crystallized as thin films on top of substrates, the resulting 2D perovskite layers do not adopt a regular growth direction parallel to the surface. Instead, the crystallites grow with no fixed orientation. As a consequence of their proximate inorganic distances and unusual crystallization tendencies, the resulting 2D perovskites exhibit low excitonic activation energies (93.59 meV and 96.53 meV, respectively), enhanced photoconductivity in solar cells, and unprecendented incident photon-to-current conversion rates of up to 60%. More importantly, mesoporous 2D layered perovskite solar cells with power conversion efficiencies (PCEs) of 1.43% and 1.83% were achieved for 1 and 2, respectively. These are the highest values obtained, thus far, for pure n = 1 lead-iodide perovskites and more than 20 times higher than those obtained for materials templated by more conventional cations, such as phenylethylammonium (0.08%).
Developing novel lanthanide metal-organic frameworks (Ln-MOFs) to rapidly and reliably differentiate both metal ions in solution and volatile organic compounds (VOCs) in vapor is highly challenging. Here, we describe versatile Eu 3+ /Tb 3+ -MOFs based on a flexible ligand. It is noteworthy that the film fabricated using bimetallic Eu 0.47 Tb 0.63 -MOF and polyvinyl alcohol could serve as an easy and convenient luminescent platform for distinguishing different metal ions and VOCs. The luminescent film exhibits notable fingerprint correlation between the metal ions/VOCs and the emission intensity ratio of Eu 3+ /Tb 3+ ions in Ln-MOFs. As a result, the bimetallic Ln-MOFs show fast recognition of Fe 3+ ion with a response time of <10 s, and can effectively probe styrene vapor within 4 min. Since the developed Ln-MOF film is stable and reliable, this work presents a promising strategy to explore luminescent platforms capable of effectively sensing different metal ions and VOCs.
The seminal discovery in 1865 by Kekulé that benzene nucleus exists with cyclic skeleton is considered to be the beginning of aromatic chemistry. Since then, a myriad of cyclic molecules displaying aromatic property have been synthesized. Meanwhile, borazine (B3N3H6), despite the isostructural and isoelectronic relationships with benzene, exhibits little aromaticity. Herein, we report the synthesis of a 1,3,2,5-diazadiborinine (B2C2N2R6) derivative, a hybrid inorganic/organic benzene, and we present experimental and computational evidence for its aromaticity. In marked contrast to the reactivity of benzene, borazine, and even azaborinines previously reported, 1,3,2,5-diazadiborinine readily forms the adducts with methyl trifluoromethanesulfonate and phenylacetylene without any catalysts. Moreover, 1,3,2,5-diazadiborine activates carbon dioxide giving rise to a bicycle[2,2,2] product, and the binding process was found to be reversible. These results, thus, demonstrate that 1,3,2,5-diazadiborinine features both nucleophilic and electrophilic boron centres, with a formal B(+I)/B(+III) mixed valence system, in the aromatic six-membered B2C2N2 ring.
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