This study is the first to demonstrate that ferroelectric R3c LiNbO3‐type ZnSnO3 nanowires (NWs), through the piezocatalysis and piezophototronic process, demonstrate a highly efficient hydrogen ...evolution reaction (HER). The polarization and electric field curves indicate that ZnSnO3 NWs exhibit typical ferroelectric hysteresis loops. Time‐resolved photoluminescence spectra reveal that the relaxation time increases with the increasing concentration of oxygen vacancies. Moderated 3H‐ZnSnO3 NWs (thermally annealed for 3 h in a hydrogen environment) have the longest extended carrier lifetime of approximately 8.3 ns. The piezoelectricity‐induced HER, via the piezocatalysis process (without light irradiation), reaches an optimal H2‐production rate of approximately 3453.1 µmol g−1 h−1. Through the synergistic piezophototronic process, the HER reaches approximately 6000 µmol g−1 in 7 h. Crucially, the mechanical force–induced spontaneous polarization functions as a carrier separator, driving the electron and hole in opposite directions in ferroelectric ZnSnO3 NWs; this separation reduces the recombination rate, enhancing the redox process. This theoretical analysis indicates that the photocatalytic and piezocatalytic effects can synergistically enhance piezophototronic performance through capitalizing on well‐modulated oxygen vacancies in ferroelectric semiconductors. This study demonstrates the essential role of this synergy in purifying water pollutants and converting water into hydrogen gas through the piezophototronic process.
The well‐controlled oxygen vacancies of ferroelectric R3c ZnSnO3 nanowires show that a highly efficient hydrogen evolution reaction (HER) reaches approximately 6000 mol g−1 in 7 h through the synergistic piezophototronic process. This is the first study to investigate how the oxygen vacancy concentration can be tuned in ferroelectric crystals to enhance the performance of piezodegradation and HER through the piezophotoelectric effect.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Linear copolymer hosts bearing a number of pillar5arene dangling side chains are synthesized for the facile construction of highly emissive supramolecular polymer networks (SPNs) upon noncovalently ...cross‐linking with a series of tetraphenyethylene (TPE)‐based tetratopic guests terminated with different functional groups through supramolecular host–guest interactions. An extremely high fluorescence quantum yield (98.22%) of the SPNs materials is obtained in tetrahydrofuran (THF) by fine‐tuning the parameters, and meanwhile supramolecular light‐harvesting systems based on spherical supramolecular nanoparticles are constructed by interweaving 9,10‐distyrylanthracene (DSA) and TPE‐based guest molecules of aggregation‐induced emission (AIE) with the copolymer hosts in the mixed solvent of THF/H2O. The present study not only illustrates the restriction of the intramolecular rotations (RIR)‐ruled emission enhancement mechanism regulated particularly by macrocyclic arene‐containing copolymer hosts, but also suggests a new self‐assembly approach to construct high‐performance light‐harvesting materials.
Supramolecular polymer networks and supramolecular nanoparticles based on copolymer hosts bearing a number of pillar5arene dangling side chains and tetraphenyethylene‐based tetratopic guests are fabricated, incorporating high fluorescence quantum yield, tunable emission wavelength, and stable microstructures. This facile strategy suggests a new self‐assembly approach to construct high‐performance light‐harvesting materials.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
3.
Desymmetrized Leaning Pillar[6]arene Wu, Jia‐Rui; Mu, Anthony U.; Li, Bao ...
Angewandte Chemie International Edition,
July 26, 2018, Volume:
57, Issue:
31
Journal Article
Peer reviewed
In this work, a novel version of macrocyclic arenes, namely leaning pillar6arenes, was discovered and it can be considered as a tilted version of a pillar6arene with two hydroxy/alkoxy ...functionalities removed. Through a facile two‐step synthetic approaches, in conjunction with a diversity of post‐modification possibilities, a series of leaning pillar6arenes, with good cavity adaptability and enhanced guest‐binding capability, was synthesized, and their self‐assembly in single‐crystal states is presented. DFT calculations demonstrated that the lower rotational barrier of unsubstituted phenylene rings, the uneven electron density centered at the leaning phenyl rings, and the polarization effect along the edge generated by the hydrogen‐bond‐induced orientation of hydroxy groups greatly affected the host‐guest properties, and meanwhile provided an intuitive explanation for the pillar‐like and rigid structure of traditional pillar6arenes. Significantly, the crystal structure of cyclo‐oligomeric quinone was obtained by direct oxidation of leaning pillar6arenes.
A lean‐to: A series of backbone‐desymmetrized pillararenes, namely leaning pillar6arenes, has been designed and successfully synthesized. They exhibit interesting three‐dimensional packing structures and enhanced host‐guest properties.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
The development of red thermally activated delayed fluorescence (TADF) emitters having excellent optoelectronic properties and satisfactory electroluminescence efficiency is full of challenges due to ...strict molecular design principles. Two red TADF molecules, 3‐(9,9‐dimethylacridin‐10(9H)‐yl)acenaphtho1,2‐bquinoxaline‐9,10‐dicarbonitrile and 3‐(2,7‐dimethyl‐10H‐spiroacridine‐9,9′‐fluoren‐10‐yl)acenaphtho1,2‐bquinoxaline‐9,10‐dicarbonitrile, are developed by adopting a donor–acceptor molecular architecture bearing an electron‐accepting acenaphtho1,2‐bquinoxaline‐9,10‐dicarbonitrile (ANQDC) moiety and a 9,9‐dimethyl‐9,10‐dihydroacridine or 2,7‐dimethyl‐10H‐spiroacridine‐9,9′‐fluorene electron donor. The combined effects of rigid and planar D/A moieties and highly steric hindrance between D and A groups endow both molecules with high rigidity to suppress nonradiative decay processes, resulting in high photoluminescence quantum efficiencies (ΦPLs) of up to 95%. Attributed to the linear and planar acceptor motif and rod‐like molecular configuration, both emitters achieve high horizontal ratios of emitting dipole orientation of ≈80%. The organic light‐emitting diodes (OLEDs) based on both emitters exhibit red emissions peaking at ≈615 nm and successfully afford ultrahigh electroluminescence performance with an external quantum efficiency of nearly 28% and a power efficiency of above 50 lm W−1, on par with the state‐of‐the‐art device efficiency for red TADF OLEDs. This presents a feasible design strategy for excellent TADF emitters simultaneously possessing high ΦPLs and horizontally aligned emitting dipoles.
An ultrahigh‐efficiency red thermally activated delayed fluorescence (TADF) OLED with an external quantum efficiency of nearly 28% and a power efficiency of exceeding 50 lm W−1 is realized. The OLEDs incorporate excellent red TADF emitters, simultaneously exhibiting 95% photoluminescence quantum efficiency and preferentially horizontal emitting dipole orientation.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Extreme temperatures are triggering and exacerbating hospital admissions and health burdens; however, it is still understudied. Therefore, we evaluated the effects of the average temperature on ...overall hospitalisation and the average length of hospital stay.
Daily area-specific age-sex stratified hospitalisation records from 2006 to 2020 were collected from the National Health Research Institutes of Taiwan. The distributed lag non-linear model was used to estimate the area-specific relative risk (RR) and 95% CI associated with daily average temperature. Overall cumulative RR was pooled from area-specific RRs using random effects meta-analysis. Temperature effects of extreme high and low thresholds were also evaluated based on the 99th (32°C) and 5th (14°C) percentiles, respectively.
Our findings suggested that the elderly (age ≥65 years) are vulnerable to temperature effects, while differential gender effects are not explicit in Taiwan. A higher risk of in-patient visits was seen among the elderly during extreme low temperatures (RR 1.08; 95% CI 1.04 to 1.11) compared with extreme high temperatures (RR 1.07; 95% CI 1.05 to 1.10). Overall, high-temperature extremes increased the risk of hospitalisation with an RR of 1.05 (95% CI 1.03 to 1.07) among the all-age-sex population in Taiwan. Additionally, lag-specific analysis of the study revealed that high-temperature effects on in-patient visits are effective on the same day of exposure, while cold effects occurred after 0-2 days of exposure. The average length of hospital stays can also increase with high-temperature extremes among age group 41-64 years and the elderly.
Public health preparedness should consider the increased load on health facilities and health expenditures during extreme temperatures.
Mechanized silica nanoparticles, equipped with pillar5arene‐2pseudorotaxane nanovalves, operate in biological media to trap cargos within their nanopores, but release them when the pH is lowered or a ...competitive binding agent is added. Although cargo size plays an important role in cargo loading, cargo charge‐type does not appear to have any significant influence on the amount of cargo loading or its release. These findings open up the possibility of using pillarnarene and its derivatives for the formation of robust and dynamic nanosystems that are capable of performing useful functions.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Synaptic dysfunction is an early pathological feature of neurodegenerative diseases associated with Tau, including Alzheimer’s disease. Interfering with early synaptic dysfunction may be ...therapeutically beneficial to prevent cognitive decline and disease progression, but the mechanisms underlying synaptic defects associated with Tau are unclear. In disease conditions, Tau mislocalizes into pre- and postsynaptic compartments; here we show that, under pathological conditions, Tau binds to presynaptic vesicles in Alzheimer’s disease patient brain. We define that the binding of Tau to synaptic vesicles is mediated by the transmembrane vesicle protein Synaptogyrin-3. In fly and mouse models of Tauopathy, reduction of Synaptogyrin-3 prevents the association of presynaptic Tau with vesicles, alleviates Tau-induced defects in vesicle mobility, and restores neurotransmitter release. This work therefore identifies Synaptogyrin-3 as the binding partner of Tau on synaptic vesicles, revealing a new presynapse-specific Tau interactor, which may contribute to early synaptic dysfunction in neurodegenerative diseases associated with Tau.
•Pathological Tau accumulates on synaptic vesicles in Alzheimer’s disease brain•Tau binds to synaptic vesicles via the transmembrane protein Synaptogyrin-3•Synaptogyrin-3 mediates Tau-induced vesicle clustering at presynaptic terminals•Synaptogyrin-3 reduction restores neurotransmitter release in fly and mouse neurons
Tau mislocalizes to presynaptic terminals in human disease conditions. Here McInnes et al. show that interaction between Tau and the presynaptic vesicle protein Synaptogyrin-3 restricts synaptic vesicle mobility, driving defects in neurotransmission in fly and mouse models of Tauopathy.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
An efficient strategy for simultaneously detecting and removing Hg2+ from water is vital to address mercury pollution. Herein a supramolecular assembly G⊂H with photoluminescent properties is ...facilely constructed through the self‐assembly of a functional pillar5arene bearing two N,N‐dimethyldithiocarbamoyl binding sites (H) and an AIE‐active tetraphenylethene derivative (G). Remarkably, the fluorescence of G⊂H can be exclusively quenched by Hg2+ among the 30 cations due to the formation of non‐luminous ground state complex and only L‐cysteine can restore fluorescence in the common 20 amino acids. Meanwhile, the probe G⊂H has a considerable thermal and pH stability, a good anti‐interference property from various cations, and a satisfactory sensitivity. More importantly, G⊂H exhibits a prominent capability of Hg2+ removal with rapid capture rate (within 1 h) and excellent adsorption efficiency (98 %), as well as a highly efficient recyclability without losing any adsorption activity.
A supramolecular functional system with appreciable photoluminescent properties on the basis of the supramolecular assembly‐induced emission enhancement (SAIEE) mechanism is successfully constructed through host‐guest interactions, which shows great potentials in simultaneously selective detection and efficient removal of Hg2+ from water owing to the formation of non‐luminous ground state complexes. This system also possesses excellent regeneration ability without the loss of adsorption activity.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
South Asia, with more than one-fifth of the world’s population, is highly vulnerable to heatwaves and associated health consequences. The population experiences considerably higher residential ...vulnerability due to limited infrastructural capacities, economic resources, and health and environmental quality deficiencies. However, a limited number of studies are available from the region to account for the health effects of heatwaves. Therefore, this study has conducted a comprehensive review to characterize heatwaves across South Asian countries. The review explicitly identifies the population’s vulnerability to heatwaves during recent years and heatwave management policies in the region. The literature review suggests increased heat-related deaths in most South Asian countries, with few exceptions. In addition, the analysis of historical temperature records identified an upward trend in annual average temperature across the South Asian countries. The study highlights various heatwave definitions that have been used in the region to facilitate comparative evidence. The review of policies identified that only a few South Asian countries have functional heatwave management plans and majorly lack community and residential preparedness for heatwaves. Therefore, this study identifies potential community- and residential-based adaptation strategies to mitigate heat discomfort. As prospective solutions, the study recommends adaptation strategies such as blue–green spaces, indoor passive cooling, infrastructural adjustments, heat action plans, etc. However, such adaptation measures require a holistic amalgamation of different stakeholders to fabricate heatwave-resilient cities.
New particle formation including atmospheric aerosol nucleation and subsequent growth, contributes to about half of cloud condensation nuclei and can grow to form haze under certain conditions, so ...its role in climate change and air quality is indispensable. However, various kinds of nucleation precursors create vast combinations of molecular clustering, hindering the understanding the detailed picture of nucleation mechanism. The recently appeared general neural network potential, ANI‐2x, covering most of elements composing nucleation clusters, looks promising to be embedded into the nucleation theoretical workflows to improve the nucleation simulation accuracy. Here we benchmarked ANI‐2x's performance on both low and high energy isomers based workflows through comparing it with semi‐empirical (PM7) and DFT (ωB97XD/6‐31++G(d,p)) methods. Results show that ANI‐2x is superior to PM7 in single point energy and geometry optimization calculations when compared against DFT. However, generally ANI‐2x's accuracy on high energy isomers is still far less than that on low energy isomers. Besides, force comparison indicates that PM7's accuracy is better than that of ANI‐2x. After all, accuracy of the workflow that focuses on low energy isomers can be benefitted from ANI‐2x while for high energy isomers based workflow, PM7 is still the better choice than ANI‐2x due to the more important role of force labels than that of energy labels in preparing machine learning dataset. However, due to the linear relation between the ANI‐2x force and DFT force, a scale factor of approximately 0.50 is expected to greatly improve the ANI‐2x force performance.
Understanding atmospheric aerosol nucleation mechanisms largely rely on theoretical calculations. Recently proposed general neural network potential, ANI‐2x, covers most of the elements in aerosol nucleation precursors, indicating a great potential to be embedded in nucleation workflows. Systematic benchmark proves the higher accuracy of ANI‐2x than PM7 in energy calculations, however, for force calculations, PM7 is a better choice despite ANI‐2x's better linear relation. After all, DFT calculations are indispensable even though PM7/ANI‐2x is utilized.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UL, UM, UPUK
PDF
