Optimising reaction conditions in flasks for performances in organic light-emitting devices.

A method for correlating reaction conditions with device performance was developed by combining Design-of-Experiments and machine-learning strategies in multistep device fabrication processes. This method allowed the "from-flask-to-device" optimisation of a macrocyclisation reaction yielding a mixture of methylated []cyclo--phenylenes, and a crude raw material was directly applied to the fabrication of Ir-doped organic light-emitting devices spin-coating. The method succeeded in eliminating energy-consuming and waste-producing separation and purification steps during device fabrication.

Sodium compensation: a critical technology for transforming batteries from sodium-starved to sodium-rich systems.

Sodium-ion batteries (SIBs) have attracted wide attention from academia and industry due to the low cost and abundant sodium resources. Despite the rapid industrialization development of SIBs, it still faces problems such as a low initial coulombic efficiency (ICE) leading to a significant decrease in battery energy density (., 20%).

Otolith radiocarbon signatures provide distinct migration history of walleye pollock around Hokkaido, Japan in the North-Western Pacific.

Trace elements and stable isotope ratios in otoliths have been used as proxies for the migration history of teleosts; however, their application in oceanic fishes remains limited. This study reports the first use of radiocarbons in otoliths to evaluate the horizontal migration histories of an oceanic fish species, the walleye pollock . We conducted radiocarbon analyses of three stocks sourced from Hokkaido, Japan.

Catalytic Nitrogen Fixation Using Well-Defined Molecular Catalysts under Ambient or Mild Reaction Conditions.

Ammonia (NH) is industrially produced from dinitrogen (N) and dihydrogen (H) by the Haber-Bosch process, although H is prepared from fossil fuels, and the reaction requires harsh conditions. On the other hand, microorganisms have fixed nitrogen under ambient reaction conditions. Recently, well-defined molecular transition metal complexes have been found to work as catalyst to convert N into NH by reactions with chemical reductants and proton sources under ambient reaction conditions.

Reversible adsorption of iridium in lyophilized cells of the unicellular red alga .

Iridium (Ir) is one of the rarest elements in the Earth's crust and is valuable in industry due to its high corrosion resistance. In this study, we used lyophilized cells of a unicellular red alga, for the selective recovery of small amounts of Ir from hydrochloric acid (HCl) solutions. The Ir recovery efficiency of the lyophilized cells was higher than that of activated carbon and comparable to that of an ion-exchange resin in up to 0.

Elucidating Conformational Dynamics and Thermostability of Designed Aromatic Clusters by Using Protein Cages.

Multiple aromatic residues assemble to form higher ordered structures known as "aromatic clusters" in proteins and play essential roles in biological systems. However, the stabilization mechanism and dynamic behavior of aromatic clusters remain unclear. This study describes designed aromatic interactions confined within a protein cage to reveal how aromatic clusters affect protein stability.

Facile Synthesis and Chiral Resolution of Expanded Helicenes with up to 35 cata-Fused Benzene Rings.

Expanded helicenes are expected to show enhanced chiroptical properties as compared to the classical helicenes but the synthesis is very challenging. Herein, we report the facile synthesis of a series of expanded helicenes Hn (n=1-4) containing 11, 19, 27 and 35 cata-fused benzene rings through Suzuki coupling-based oligomerization followed by Bi(OTf) -mediated regioselective cyclization of vinyl ethers. Their structures were determined by X-ray crystallographic analysis.

Residual Neuropathic Pain in Postoperative Patients With Cervical Ossification of Posterior Longitudinal Ligament.

Study Design: A prospective multi-institutional observational study.

Objective: To investigate and identify risk factors for residual neuropathic pain after surgery in patients with cervical ossification of posterior longitudinal ligament (c-OPLL).

Summary Of Background Data: Patients with c-OPLL often require surgery for numbness and paralysis of the extremities; however, postoperative neuropathic pain can considerably deteriorate their quality of life.

Reentrant 2D Nanostructured Liquid Crystals by Competition between Molecular Packing and Conformation: Potential Design for Multistep Switching of Ionic Conductivity.

Reentrant phenomena in soft matter and biosystems have attracted considerable attention because their properties are closely related to high functionality. Here, we report a combined experimental and computational study on the self-assembly and reentrant behavior of a single-component thermotropic smectic liquid crystal toward the realization of dynamically functional materials. We have designed and synthesized a mesogenic molecule consisting of an alicyclic trans,trans-bicyclohexyl mesogen and a polar cyclic carbonate group connected by a flexible tetra(oxyethylene) spacer.

Modular synthesis, host-guest complexation and solvation-controlled relaxation of nanohoops with donor-acceptor structures.

Carbon nanohoops with donor-acceptor (D-A) structures are attractive electronic materials and biological fluorophores, but their synthesis is usually challenging. Moreover, the preparation of D-A nanohoop fluorophores exhibiting high fluorescence quantum yields beyond 500 nm remains a key challenge. This study presents a modular synthetic approach based on an efficient metal-free cyclocondensation reaction that readily produced nine congeners with D-A or donor-acceptor-donor' (D-A-D') structures, one of which is water-soluble.

Association between meal frequency with others and psychological distress during the COVID-19 pandemic: A cross-sectional study.

Aim: Previous studies evaluated the association between eating alone and mental health mainly in older people and adolescents. This study aimed to evaluate the association between dinner frequency with others and psychological distress during the COVID-19 outbreak among the Japanese working population.

Methods: Data were acquired from a prospective online cohort study (the Employee Cohort Study in the COVID-19 pandemic in Japan) conducted in February 2021 as a cross-sectional design.

Free water derived by multi-shell diffusion MRI reflects tau/neuroinflammatory pathology in Alzheimer's disease.

Introduction: Free-water (FW) imaging, a new analysis method for diffusion magnetic resonance imaging (MRI), can indicate neuroinflammation and degeneration. We evaluated FW in Alzheimer's disease (AD) using tau/inflammatory and amyloid positron emission tomography (PET).

Methods: Seventy-one participants underwent multi-shell diffusion MRI, F-THK5351 PET, C-Pittsburgh compound B PET, and neuropsychological assessments.

Ruthenium- and Copper-Catalyzed Propargylic Substitution Reactions of Propargylic Alcohol Derivatives with Hydrazones.

Ruthenium- and copper-catalyzed propargylic substitution reactions of propargylic alcohol derivatives with N-monosubstituted hydrazones as ambident nucleophiles are achieved in which N-monosubstituted hydrazones exhibit impressive different reactivities depending on different catalytic systems, behaving as carbon-centered nucleophiles to give the corresponding propargylic alkylated products in ruthenium catalysis, or as nitrogen-centered nucleophiles to afford the corresponding propargylic aminated products in copper catalysis. DFT calculations were carried out to investigate the detailed reaction pathways of these two systems. Further transformation of propargylic substituted products affords the corresponding multisubstituted pyrazoles as cyclization products in good to high yields.

Optimal water concentration for aqueous Li intercalation in vanadyl phosphate.

Development of high-performance aqueous batteries is an important goal for energy sustainability owing to their environmental benignity and low fabrication costs. Although a layered vanadyl phosphate is one of the most-studied host materials for intercalation electrodes with organic electrolytes, little attention has been paid to its use in aqueous Li systems because of its excessive dissolution in water. Herein, by controlling the water concentration, we demonstrate the stable operation of a layered vanadyl phosphate electrode in an aqueous Li electrolyte.

Nanostructured liquid-crystalline Li-ion conductors with high oxidation resistance: molecular design strategy towards safe and high-voltage-operation Li-ion batteries.

Nanostructured, uncharged liquid-crystalline (LC) electrolyte molecules having bicyclohexyl and cyclic carbonate moieties have been developed for application in Li-ion batteries as quasi-solid electrolytes, which suppress leakage and combustion. Towards the development of safe and high performance Li-ion batteries, we have designed Li-ion conductive LC materials with high oxidation resistance using density functional theory (DFT) calculation. The DFT calculation suggests that a mesogen with a bicyclohexyl moiety is suitable for the high-oxidation-resistance LC electrolytes compared to a mesogen containing phenylene moieties.

Self-activated Rh-Zr mixed oxide as a nonhazardous cocatalyst for photocatalytic hydrogen evolution.

Efficient, robust and environmentally friendly cocatalysts for photocatalysts are important for large-scale solar hydrogen production. Herein, we demonstrate that a Rh-Zr mixed oxide is an efficient cocatalyst for hydrogen evolution. Impregnation of Zr and Rh precursors (Zr/Rh = 5 wt/wt%) formed RhZrO cocatalyst particles on Al-doped SrTiO, which exhibited 31× higher photocatalytic water-splitting activity than a RhO cocatalyst.

Self-healing and shape memory functions exhibited by supramolecular liquid-crystalline networks formed by combination of hydrogen bonding interactions and coordination bonding.

We here report a new approach to develop self-healing shape memory supramolecular liquid-crystalline (LC) networks through self-assembly of molecular building blocks combination of hydrogen bonding and coordination bonding. We have designed and synthesized supramolecular LC polymers and networks based on the complexation of a forklike mesogenic ligand with Ag ions and carboxylic acids. Unidirectionally aligned fibers and free-standing films forming layered LC nanostructures have been obtained for the supramolecular LC networks.

Stereoretentive N-Arylation of Amino Acid Esters with Cyclohexanones Utilizing a Continuous-Flow System.

The N-arylation of chiral amino acid esters with minimal racemization is a challenging transformation because of the sensitivity of the α-stereocenter. A versatile synthetic method was developed to prepare N-arylated amino acid esters using cyclohexanones as aryl sources under continuous-flow conditions. The designed flow system, which consists of a coil reactor and a packed-bed reactor containing a Pd(OH) /C catalyst, efficiently afforded the desired N-arylated amino acids without significant racemization, accompanied by only small amounts of easily removable co-products (i.

Lévy Walk in Swarm Models Based on Bayesian and Inverse Bayesian Inference.

While swarming behavior is regarded as a critical phenomenon in phase transition and frequently shows the properties of a critical state such as Lévy walk, a general mechanism to explain the critical property in swarming behavior has not yet been found. Here, we address this problem with a simple swarm model, the Self-Propelled Particle (SPP) model, and propose a way to explain this critical behavior by introducing agents making decisions via the data-hypothesis interaction in Bayesian inference, namely, Bayesian and inverse Bayesian inference (BIB). We compare three SPP models, namely, the simple SPP, the SPP with Bayesian-only inference (BO) and the SPP with BIB models.

Welcome to the 2020 Tateshina Conference on Organic Chemistry!

In his editorial, Shū Kobayashi is expressing his welcome to the 2020 Tateshina Conference on Organic Chemistry. This year the conference cannot take place at Kurumayama Kogen Sky Park but is held as a paper meeting in the form of a special collection of Chemistry - An Asian Journal.

Acyclic, Linear Oligo-meta-phenylenes as Multipotent Base Materials for Highly Efficient Single-layer Organic Light-emitting Devices.

Oligo-meta-phenylenes have been designed and synthesized as multipotent base materials of single-layer organic light-emitting devices. Simple molecular structures of oligo-meta-phenylenes composed of linear phenylene arrays benefited from the wealth of modern reactions available for biaryl couplings and were concisely synthesized in a series. Structure-performance relationship studies with the first seven congeners revealed key features important for the multipotent materials in single-layer devices.

Direct and quantitative monitoring of catalytic organic reactions under heterogeneous conditions using direct analysis in real time mass spectrometry.

This new method overcomes problems of conventional analytical methodologies such as light scattering and sampling reproducibility issues. We used this method for mechanistic studies of catalytic reactions under heterogeneous conditions. Direct-type hydroxymethylation reactions and Mukaiyama-type hydroxymethylation reactions both catalyzed by a scandium-bipyridine ligand complex under micellar conditions were employed as examples of heterogeneous reactions.

Synthesis of 1,2,4-azadiphosphole derivatives based on vanadium-catalyzed [2+2+1] cycloaddition reactions of azobenzenes with phosphaalkynes.

A new synthetic method is described to construct 1,2,4-azadiphosphole derivatives based on vanadium-catalyzed [2+2+1] cycloaddition reactions. Reactions of azobenzenes as nitrogen sources with phosphaalkynes as phosphorous counterparts in the presence of VCl(thf) as a catalyst afford the corresponding 1,2,4-azadiphospholes.