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Epidemiologic findings indicate that unfavorable cardiovascular (CV) risk profiles, such as elevated systolic blood pressure (SBP), low-density lipoprotein cholesterol (LDL-C), and overweight, decelerate with aging. Few studies, however, have evaluated the association between the CV risk profile and frailty. We performed a cross-sectional analysis using the baseline data of a prospective cohort study. A total of 599 subjects (age, 78 [range 70-83] years; men, 50%) were analyzed in an outpatient setting. Frailty was diagnosed in 37% of the patients according to the Kihon Checklist score. An unfavorable CV risk profile was associated with a lower risk of frailty. The adjusted odds ratios (ORs; 95% confidence interval [CI]) of each CV risk factor for frailty were as follows SBP (each 10 mmHg increase) 0.83 (0.72-0.95), LDL-C (each 10 mg/dl increase) 0.96 (0.86-1.05), and body mass index (each 1 kg/m2 increase) 1.03 (0.97-1.10). Moreover, the total number of CV risk factors within the optimal range was significantly associated with the risk of frailty with the following ORs (95% CI) 1, 2.30 (0.75-8.69); 2, 3.22 (1.07-11.97); and 3, 4.79 (1.56-18.05) compared with patients having no risk factors within optimal levels (p for trend 0.008). Abnormal homeostasis might lead to lower levels of CV risk factors, which together result in "reverse metabolic syndrome." Our findings indicate that a favorable CV risk profile is associated with frailty.Blood pressure (BP) is one of the most dynamic physiologic variables that is routinely measured in clinical practice and is characterized by continuous and significant changes beat-to-beat, over 24 h, day-to-day, and visit-to-visit. Under physiological conditions, these BP variations largely represent a response to environmental stimulations and challenges of daily life aimed at maintaining so-called cardiovascular "homeostasis". However, sustained increases in blood pressure variability (BPV) may also reflect alterations in cardiovascular regulatory mechanisms or underlying pathological conditions and may represent a source of damage to the cardiovascular system. The clinical significance and prognostic implications of these BP variations have been demonstrated by a series of clinical and population studies conducted in recent years, in which increasing BPV has been associated with a higher risk of subclinical organ damage, cardiovascular events, and cardiovascular and all-cause mortality, independent of elevated average BP values. This paper will review the available evidence on the current definitions, classification, and mechanisms responsible for different types of BPV by focusing on their relevance to cardiovascular homeostasis and cardiovascular disease.This article focuses on selected large prospective cohort studies that examined the effect of alcohol consumption on the risks of hypertension and cardiovascular disease in Japanese men and women. Regardless of age and sex, alcohol consumption was positively associated with an increased risk of hypertension. selleck inhibitor There was a J-shaped association between alcohol consumption and the risks of stroke and cardiovascular disease in Japanese men, which was consistent with the findings of the studies conducted by Western countries. Few studies have been conducted to examine the effect of alcohol consumption on the risks of stroke and coronary heart disease in Asian women. We first showed that heavy alcohol consumption of ≥300 g ethanol/week was associated with increased risk of total stroke, hemorrhagic stroke, intraparenchymal hemorrhage, subarachnoid hemorrhage and ischemic stroke in women while light drinking was not associated with a reduced risk of stroke. Furthemore, heavy drinking (≥46.0 g ethanol/day) had an increased risk of mortality from coronary heart disease in women, whereas light drinking (0.1-22.9 g ethanol/day) had a reduced risk of mortality from total cardiovascular disease. The association between alcohol consumption and the risk of stroke was modified by social support and salt preference.The Soai reaction has profoundly impacted chemists' perspective of autocatalysis, chiral symmetry breaking, absolute asymmetric synthesis and its role in the origin of biological homochirality. Here we describe the unprecedented observation of asymmetry-amplifying autocatalysis in the alkylation of 5-(trimethylsilylethynyl)pyridine-3-carbaldehyde using diisopropylzinc. Kinetic studies with a surrogate substrate and spectroscopic analysis of a series of zinc alkoxides that incorporate specific structural mutations reveal a 'pyridine-assisted cube escape'. The new tetrameric cluster functions as a catalyst that activates the substrate through a two-point binding mode and poises a coordinated diisopropylzinc moiety for alkyl group transfer. Transition-state models leading to both the homochiral and heterochiral products were validated by density functional theory calculations. Moreover, experimental and computational analysis of the heterochiral complex provides a definitive explanation for the nonlinear behaviour of this system. Our deconstruction of the Soai system reveals the structural logic for autocatalyst evolution, function and substrate compatibility-a central mechanistic aspect of this iconic transformation.ortho-Quinone methides are useful transient synthetic intermediates in organic synthesis. These species are most often generated in situ by the acid- or base-mediated transformation of phenols that have been pre-functionalized at a benzylic position, or by biomimetic oxidation of the corresponding ortho-alkylphenols with metal oxidants or transition-metal complexes. Here we describe a method for the transition-metal-free oxidative generation of o-QMs from ortho-alkylarenols, using hypoiodite catalysis under nearly neutral conditions, which can then be applied in one-pot tandem reactions. This method for the chemoselective oxidative generation of ortho-quinone methides may prove superior to previous methods with respect to environmental issues and scope, and can be applied to various tandem reactions such as inter- or intramolecular [4 + 2] cycloaddition, oxa-6π-electrocyclization, conjugate addition and spiroepoxidation.The introduction of a trifluoromethyl (CF3) group can dramatically improve a compound's biological properties. Despite the well-established importance of trifluoromethylated compounds, general methods for the trifluoromethylation of alkyl C-H bonds remain elusive. Here we report the development of a dual-catalytic C(sp3)-H trifluoromethylation through the merger of light-driven, decatungstate-catalysed hydrogen atom transfer and copper catalysis. This metallaphotoredox methodology enables the direct conversion of both strong aliphatic and benzylic C-H bonds into the corresponding C(sp3)-CF3 products in a single step using a bench-stable, commercially available trifluoromethylation reagent. The reaction requires only a single equivalent of substrate and proceeds with excellent selectivity for positions distal to unprotected amines. To demonstrate the utility of this new methodology for late-stage functionalization, we have directly derivatized a broad range of approved drugs and natural products to generate valuable trifluoromethylated analogues. Preliminary mechanistic experiments reveal that a 'Cu-CF3' species is formed during this process and the critical C(sp3)-CF3 bond-forming step involves the copper catalyst.Advances in chemical control of the photophysical properties of transition-metal complexes are revolutionizing a wide range of technologies, particularly photocatalysis and light-emitting diodes, but they rely heavily on molecules containing precious metals such as ruthenium and iridium. Although the application of earth-abundant 'early' transition metals in photosensitizers is clearly advantageous, a detailed understanding of excited states with ligand-to-metal charge transfer (LMCT) character is paramount to account for their distinct electron configurations. Here we report an air- and moisture-stable, visible light-absorbing Zr(IV) photosensitizer, Zr(MesPDPPh)2, where [MesPDPPh]2- is the doubly deprotonated form of [2,6-bis(5-(2,4,6-trimethylphenyl)-3-phenyl-1H-pyrrol-2-yl)pyridine]. This molecule has an exceptionally long-lived triplet LMCT excited state (τ = 350 μs), featuring highly efficient photoluminescence emission (Ф = 0.45) due to thermally activated delayed fluorescence emanating from the higher-lying singlet configuration with significant LMCT contributions. Zr(MesPDPPh)2 engages in numerous photoredox catalytic processes and triplet energy transfer. Our investigation provides a blueprint for future photosensitizer development featuring early transition metals and excited states with significant LMCT contributions.Ionic conductors serve as solid electrolytes for fuel cells and batteries, whereas polar crystals such as ferroelectrics and pyroelectrics-which are typically insulating materials-are used in electronic devices. Here we show a material that combines superionic conductivity with a polar crystal structure at room temperature. This three-dimensional anionic network is based on -Fe-N≡C-Mo- units, with Cs cations hosted in every other pore. In the resulting Cs1.1Fe0.95[Mo(CN)5(NO)]·4H2O material, the negative and positive charges of the framework and Cs+ ions, respectively, are non-symmetrically shifted in the c-axis direction of the unit cell, and spontaneous electric polarization is generated, in turn leading to second harmonic generation (SHG). Additionally, this material is a superionic conductor (with an ionic conductivity value of 4 × 10-3 S cm-1 at 318 K). Furthermore, the ionic conductivity significantly decreases under 532 nm light irradiation (from 1 × 10-3 S cm-1 to 6 × 10-5 S cm-1 at room temperature) and, when irradiation stops, returns to its original value within ~1 h.Electronic symmetry breaking by charge disproportionation results in multifaceted changes in the electronic, magnetic and optical properties of a material, triggering ferroelectricity, metal/insulator transition and colossal magnetoresistance. Yet, charge disproportionation lacks technological relevance because it occurs only under specific physical conditions of high or low temperature or high pressure. Here we demonstrate a voltage-triggered charge disproportionation in thin molecular films of a metal-organic complex occurring in ambient conditions. This provides a technologically relevant molecular route for simultaneous realization of a ternary memristor and a binary memcapacitor, scalable down to a device area of 60 nm2. Supported by mathematical modelling, our results establish that multiple memristive states can be functionally non-volatile, yet discrete-a combination perceived as theoretically prohibited. Our device could be used as a binary or ternary memristor, a binary memcapacitor or both concomitantly, and unlike the existing 'continuous state' memristors, its discrete states are optimal for high-density, ultra-low-energy digital computing.Lysosomes have become an important target for anticancer therapeutics because lysosomal cell death bypasses the classical caspase-dependent apoptosis pathway, enabling the targeting of apoptosis- and drug-resistant cancers. However, only a few small molecules-mostly repurposed drugs-have been tested so far, and these typically exhibit low cancer selectivity, making them suitable only for combination therapies. Here, we show that mixed-charge nanoparticles covered with certain ratios of positively and negatively charged ligands can selectively target lysosomes in cancerous cells while exhibiting only marginal cytotoxicity towards normal cells. This selectivity results from distinct pH-dependent aggregation events, starting from the formation of small, endocytosis-prone clusters at cell surfaces and ending with the formation of large and well-ordered nanoparticle assemblies and crystals inside cancer lysosomes. These assemblies cannot be cleared by exocytosis and cause lysosome swelling, which gradually disrupts the integrity of lysosomal membranes, ultimately impairing lysosomal functions and triggering cell death.