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© 2020 The Authors. Head & Neck published by Wiley Periodicals, Inc.The alkylation of amines by alcohols is a broadly applicable, sustainable, and selective method for the synthesis of alkyl amines, which are important bulk and fine chemicals, pharmaceuticals, or agrochemicals. Here we report that Cr complexes can catalyze this C-N bond formation reaction. We synthesized and isolated 35 examples of alkylated amines. Thirteen previously undisclosed products could be obtained and the use of amino alcohols as alkylating agents could be demonstrated. The catalyst tolerates numerous functional groups, among them hydrogenation sensitive examples. In comparison to many other alcohol-based amine alkylation protocols where a stoichiometric amount of base is required, our Cr based catalyst system permits product isolation with yields higher than 90% for various alkyl amines with a catalytic amount of base only. Our study indicates that Cr complexes can catalyze borrowing hydrogen or hydrogen auto-transfer reactions and, thus, could be an alternative to Fe, Co and Mn or noble metals in (de)hydrogenation catalysis. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.Molecular recognition in cell biological process is characterized with specific locks-and-keys interactions between ligands and receptors, but which are ubiquitously distributed on cell membrane with topological clustering. Few topologically-engineered ligand systems enable the exploration of the binding strength between ligand-receptor topological organization. Here we generate topologically controlled ligands by developing a family of tetrahedral DNA frameworks (TDFs), so the multiple ligands are stoichiometrically and topologically arranged. This topological control of multiple ligands changes the nature of the molecular recognition by inducing the receptor clustering, so the binding strength is significantly improved (~10-fold). The precise engineering of topological complexes formed by the TDFs are readily translated into effective binding control for cell patterning and binding strength control of cells for cell sorting. This work paves the way for the development of versatile design of topological ligands with potential applications for cell recognition and cell communication. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.BACKGROUND Intellectual disabilities and autism are lifelong and often co-occur. Little is known on their extent of independent association with sensory impairments and physical disability. METHODS For Scotland's population, logistic regressions investigated age-gender-adjusted odds ratios (OR) of associations, independently, of intellectual disabilities and autism with sensory impairments and physical disability. RESULTS 1,548,819 children/youth, and 3,746,584 adults. In children/youth, the effect size of intellectual disabilities and autism, respectively, was as follows blindness (OR = 30.12; OR = 2.63), deafness (OR = 13.98; OR = 2.31), and physical disability (OR = 43.72; OR = 5.62). For adults, the effect size of intellectual disabilities and autism, respectively, was as follows blindness (OR = 16.89; OR = 3.29), deafness (OR = 7.47; OR = 2.36), and physical disability (OR = 6.04; OR = 3.16). CONCLUSIONS Intellectual disabilities have greater association with the population burden of sensory impairments/physical disability, but autism is also associated regardless of overlap with intellectual disabilities. These may impact further on communication limitations due to autism and intellectual disabilities, increasing complexity of assessments/management of other health conditions. Clinicians need to be aware of these important issues. © 2020 The Authors. Journal of Applied Research in Intellectual Disabilities published by John Wiley & Sons Ltd.Nests of three silanol groups are located on the internal pore surface of calcined zeolite SSZ-70. 2D 1H double/triple-quantum single-quantum correlation NMR experiments enable a rigorous identification of these silanol triad nests. They reveal a close proximity to the structure directing agent (SDA), that is N,N'-diisobutyl imidazolium cations, in the as-synthesized material, where the defects are negatively charged (silanol dyad plus one charged SiO¯ siloxy group) for charge balance. It is inferred that ring strain prevents the condensation of silanol groups upon calcination and removal of the SDA to avoid energetically unfavorable three-rings. In contrast, tetrad nests, created by boron extraction from B-SSZ-70 at various other locations, are not stable and silanol condensation occurs. Infrared spectroscopic investigations of adsorbed pyridine indicate an enhanced acidity of the silanol triads, suggesting important implications in catalysis. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.Lemborexant is a dual orexin receptor antagonist indicated for the treatment of adult and elderly individuals with insomnia. Some current pharmacologic treatments for insomnia cause respiratory depression, a serious safety concern, particularly for individuals with obstructive sleep apnea (OSA). This phase 1, randomized, double-blind, placebo-controlled, two-period crossover study examined respiratory safety parameters in individuals with mild OSA following treatment with lemborexant. Participants (n = 39) were randomized to one of two treatment sequences, including placebo and lemborexant 10 mg. Each treatment period lasted 8 days and was separated by a washout of at least 14 days. Following single or multiple doses, there were no significant differences in mean apnea-hypopnea index for lemborexant 10 mg versus placebo (least squares mean [LSM] difference [95% confidence interval CI] day 1, -0.03 [-2.22, 2.17]; day 8, -0.06 [-1.95, 1.83]) or peripheral capillary oxygen saturation during sleep (LSM difference [95% CI] day 1, 0.07 [-0.31, 0.46]; day 8, 0.25 [-0.11, 0.61]). There were no significant differences versus placebo for the percentage of total sleep time during which peripheral capillary oxygen saturation was less then 80% (LSM difference [95% CI] day 1, 0.002 [-0.019, 0.023]; day 8, 0.006 [-0.015, 0.026]), less then 85% (LSM difference [95% CI] day 1, 0.067 [-0.124, 0.258]; day 8, 0.056 [-0.117, 0.228]) or less then 90% (LSM difference [95% CI] day 1, 0.312 [-0.558, 1.181]; day 8, 0.088 [-0.431, 0.607]). The incidence of treatment-emergent adverse events was low and similar for lemborexant and placebo. Lemborexant demonstrated respiratory safety in this study population and was well tolerated. © 2020 The Authors. Journal of Sleep Research published by John Wiley & Sons Ltd on behalf of European Sleep Research Society.Synthesis of fully conjugated cyclophanes containing large-size polycyclic aromatics is a challenging task. Herein, we report the synthesis of three benzidine linked, hexa-peri-hexabenzocoronene (the so-called "superbenzene") based ortho- (1-NH), para- (2-NH), and meta- (3-NH) cyclophanes through intermolecular Yamamoto coupling reaction of structurally pre-organized precursors. Subsequent oxidative dehydrogenation gave the corresponding quinoidal benzidine linked cyclophanes 1-N, 2-N and 3-N. Their geometries were confirmed by X-ray crystallographic analysis and their electronic properties were investigated by electronic absorption, cyclic voltammetry, and DFT calculations. The quinoidal benzidine-linked cyclophanes all show thermally populated paramagnetic activity with a relatively large singlet-triplet energy gap. The structure-property relationship was discussed. Two enantiomers for the ortho- cyclophanes (1-NH and 1-N) were isolated by chiral HPLC and their chiral figure-of-eight macrocyclic structures were identified by X-ray analysis and circular dichroism spectral measurements. The cage-like cyclophanes 2-NH and 3-NH with concave surface can selectively encapsulate fullerene C70 with an association constant Ka of 1.95×105 M-1 and 5.51×104 M-1, respectively. © 2020 WILEY-VCH Verlag GmbH & Co. CC-885 research buy KGaA, Weinheim.Very recently, hydrovoltaic technology is emerging as a novel renewable energy harvesting method through carefully controlling the interaction between water and solid surface, which dramatically extends the capability to harvest water energy. However, the urgent issue restricting its device performance is poor carrier transport properties of the solid surface if large charged interface is considered simultaneously. Here, a hydrovoltaic device based on silicon nanowire arrays (SiNWs), which provide large charged surface/volume ratio and excellent carrier transport properties simultaneously, yields sustained electricity via carrier concentration gradient induced by evaporation-induced water flow inside nanochannels. And a device can yield direct current with a short-circuit current density of over 55 μA/cm 2 , which is three orders larger than previous reported analogous device (approximately 40 nA/cm 2 ). In addition, this device exhibits a constant output power density of over 6 μW/cm 2 and an open-circuit voltage of up to 400 mV, which enables it to easily drive a commercial light emitting diode. We also demonstrate the potential application of this electrokinetic phenomenon by using it to create a breathing sensor. Through changing ion concentration in water, length and surface charge of SiNWs, we propose the mechanism of harvesting energy through water flow in SiNWs. Our findings reveal that the generated energy should be mainly correlated with Debye screening effect and Coulomb interactions. Our finding may pave a way for developing innovative energy-harvesting devices from ubiquitous evaporation-driven internal water flow in nature with semiconductor material of silicon. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.Tumor microenvironment (TME) are vital components of tumor tissue. Increasing evidence suggest their significance in predicting outcomes and guiding therapies. However, no studies have reported a systematic analysis of clinicopathological significance of TME in lung adenocarcinoma (LUAD). Here, we inferred tumor stromal cells in 1,184 LUAD patients using computational algorithms based on bulk tumor expression data, and evaluated clinicopathological significance of stromal cells. We found LUAD patients showed heterogeneous abundance in stromal cells. Infiltration of stromal cells was influenced by clinicopathological features, such as age, gender, smoking and TNM stage. By clustering stromal cells, we identified two clinically and molecularly distinct LUAD subtypes with immune active and immune repressed features. The immune active subtype is characterized with repressed metabolism and repressed proliferation of tumor cells, while the immune repressed subtype is characterized with active metabolism and active proliferation of tumor cells. Differentially expressed gene analysis of the two LUAD subtypes identified an immune-activation signature. To diagnose TME subtypes practically, we constructed TME score using principal component analysis based on the immune-activation signature. The TME score predicted TME subtypes effectively in three independent datasets with areas under the curves (AUCs) of 0.960, 0.812, and 0.819, respectively. In conclusion, we proposed two clinically and molecularly distinct LUAD subtypes based on tumor microenvironment that may be valuable in predicting clinical outcome and guiding immunotherapy. This article is protected by copyright. All rights reserved.
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