Abstract Recent technological advancements encompassed under the Mobile Brain/Body Imaging (MoBI) framework https://paperpile.com/c/Y9SL6l/8NAW5(Makeig et al., 2009), have produced exciting new experimental results linking mind, brain, and behavior https://paperpile.com/c/Y9SL6l/qjBlh+HHrGy+uTqfJ(Gramann et al., 2014; Ladouce et al., 2017; Shamay‐Tsoory & Mendelsohn, 2019). The main goal of the MoBI approach is to model brain and body dynamics during every‐day, natural, real‐life situations.
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ABSTRACT Background Asthma is heterogeneous disease with different phenotypes, endotypes, and severities. Definition of these subgroups requires the identification of biomarkers in biological samples, and serum proteomics is a useful and minimally invasive method for this purpose. Therefore, the aim of this study was to detect serum proteins whose abundance is distinctively associated with different asthma phenotypes (allergic vs. non‐allergic) or severities. Methods For each group of donors...
Abstract Background Chronic rhinosinusitis (CRS) is a chronic inflammatory disease associated with a substantial personal and socio‐economic burden. Monitoring of patient‐reported outcomes by mobile technology offers the possibility to better understand real‐life burden of CRS. Methods This study reports on the cross‐sectional evaluation of data of 626 users of mySinusitisCoach (mSC), a mobile application for CRS patients. Patient characteristics of mSC users were analysed as well as the...
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Salivary duct carcinoma (SDC) is an aggressive subtype of primary salivary gland carcinoma, often with an advanced stage at presentation and high rates of metastasis and recurrence. It most commonly arises in the parotid gland of older men and microscopically resembles high‐grade breast ductal carcinoma. While 50 years have lapsed since the first report of this entity, recent intensive studies have shed light on its biologic, genetic, and clinical characteristics. The diagnosis of SDC is aided by...
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Neoplastic or dysplastic neuronal tissue in the brain stem and cerebellum can become epileptogenic in pediatric patients. However, it is unknown whether such tissue may transform intrinsic properties of the human cerebellum, making it capable of generating epileptic population activity. We noninvasively detected epileptiform signals unaveraged in a pediatric patient with epilepsy due to a tumor in the middle cerebellar peduncle. Analysis of generators of the signals revealed that the cerebellum ipsi‐...
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Abstract Lemierre syndrome is septic thrombophlebitis in the internal jugular vein due to oropharyngeal bacterial infection. The most frequent culprit is the gram negative anaerobe Fusobacterium necrophorum. The syndrome has its name from André‐Alfred Lemierre (1875‐1956), professor in bacteriology in Paris, who in 1936 published a case series of 20 patients with fatal outcome in 18 (90%).[1] At the time when Lemierre described the disease it was much more common than presently. Sibai and Sarasin...
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Commercially available, classic Noyori RuII‐diamine‐diphosphine catalysts catalyze the cross coupling of racemic secondary alcohols with primary alcohols in the presence of a base, affording new chiral alcohols with enantiomeric ratios of up to 99:1. Abstract The first example of an asymmetric Guerbet reaction has been developed. Using commercially available, classic Noyori RuII‐diamine‐diphosphine catalysts, well‐known in asymmetric hydrogenation, racemic secondary alcohols are shown to couple...
New approach to lithium–sulfur batteries: A trilayer MoN‐C‐MoN sandwich structure characterized by a continuous 2D catalysis–conduction contact interface was prepared as a sulfur cathode host. The two MoN outer layers adsorb LiPSs/Li2S2/Li2S products and accelerate their conversion, while the C interlayer acts as a high‐flux electron transfer pathway to reinforce the overall conductivity of the sandwich structure. In this way the accumulation of dead Li2S2/Li2S can be avoided even after extended...
Two diterpene synthases from the bacterial genus Chryseobacterium making the new compounds chryseodiene and wanjudiene are reported. The enzyme mechanisms were investigated in detail through a combination of experimental and computational approaches. Abstract Two bacterial diterpene synthases (DTSs) from Chryseobacterium were characterised. The first enzyme yielded the new compound chryseodiene that closely resembles the known fusicoccane diterpenes from fungi, but its experimentally and computationally...
Rigidity leads to inertness: The 2,4‐pyridyl‐disubstituted bispidol ligand L1 is a promising structural entry for the development of Mn‐based imaging agents. Thanks to its preorganized rigid structure, it provides exceptional inertness to the Mn2+ complex. MnL1 is monohydrated, has good relaxation efficiency for MRI applications, and undergoes rapid renal clearance when injected into mice. The 52Mn‐labeled radiocomplex could be obtained and was stable in biological media. Abstract The search...
Paramagnetic CoII complexes produce water 1H shifts that rival those of lanthanide(III) complexes. Incorporation of these complexes into the interior and bilayer of shrunken liposomes gives highly shifted intraliposomal water protons for chemical exchange saturation transfer (CEST) experiments as the first examples of transition metal ion lipoCEST agents. Abstract Three paramagnetic CoII macrocyclic complexes containing 2‐hydroxypropyl pendant groups, 1,1′,1′′,1′′′‐(1,4,8,11‐tetraazacyclotetradecane‐1,4,8,11‐tetrayl)tetrakis‐...
Unstrained melody: A photo‐promoted skeletal rearrangement reaction of phosphine–borane frustrated Lewis pairs, o‐(borylaryl)phosphines, involving cleavage of an unstrained sp2C–sp3C σ‐bond is reported. The reaction realizes an efficient synthesis of cyclic phosphonium borate compounds. The reaction mechanism via a boranorcaradiene intermediate is proposed based on calculations. Abstract An unprecedented photo‐promoted skeletal rearrangement reaction of phosphine–borane frustrated Lewis pairs,...
Here, we report surface‐enhanced Raman scattering‐chiral anisotropy (SERS‐ChA) effect that combines chiral discrimination and surface Raman scattering enhancement on chiral nanostructured Au films (CNAFs) equipped in the normal Raman scattering Spectrometer. The CNAFs provided remarkably higher enhancement factors of Raman scattering (EFs) for particular enantiomers, and the SERS intensity was proportional to the enantiomeric excesses ( ee) values. Except for molecules with mesomeric species, all...
Weak binding of hydrogen atoms to the 2H‐MoS 2 basal plane renders MoS 2 inert as an electrocatalyst for the hydrogen evolution reaction. Transition metal doping can activate neighboring sulfur atoms in the MoS 2 basal plane to bind hydrogen more strongly. Our density functional theory‐based studies show strong variation in the degree of activation by dopants across the 3d transition metal series (Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn). To understand the trends in activation, we propose a theoretical...
Electrochemical reduction of CO2 to valuable fuels is appealing for CO2 fixation and energy storage. However, the development of electrocatalysts with high activity and selectivity in a wide potential window is challenging. Herein, atomically thin bismuthene (Bi‐ene) is pioneeringly obtained via an in situ electrochemical transformation process from ultrathin bismuth‐based metal–organic layers. The few‐layer Bi‐ene, which possesses a great mass of exposed active sites with high intrinsic activity,...
Here we disclose a cobaloxime‐catalyzed acceptorless dehydrogenative cyclization of o ‐teraryls. In stark contrast to the established methods such as the Scholl or Mallory reactions, this protocol does not require any strong acids or oxidants, showing high atom economy and a broad substrate scope. It operates at near room temperature with light as the source of energy. Acid or oxidant‐sensitive functional groups, such as 4‐methoxyphenyl, unprotected benzyl alcohol, silyl ether and thiophene, are...
An engineered iodine catalysis for the light‐promoted homolytic C‐H bond cleavage provides straightforward access to aliphatic fluorination. The intermediary formation of amidyl radicals enables selective C‐H functionalization via carbon‐centered radicals. For the subsequent C‐F bond formation, previous methodology is typically limited to the use of electrophilic fluorine reagents. We here demonstrate that the intermediary instalment of a carbon‐iodine bond sets the strategic basis for an Umpolung...
In this study, we demonstrate the concept of ‘reverse design’ for virus inhibitors. With the current knowledge of influenza A virus (IAV), we designed a nano‐inhibitor that has a reverse shape to the viral particle and heteromultivalent inhibitory effects on hemagglutinin and neuraminidase. The synthesized nano‐inhibitor can neutralize the viral particle extracellularly and block its attachment and entry to the host cells. The virus replication was significantly reduced by 6 orders of magnitude in...
The site‐selective “cut and sew” transformations employing diazo compounds and hypervalent iodine(III) compounds involve the departure of leaving groups, a “cut” process, followed by reorganizing of fragments by bond connections, a “sew” process. Bearing controllable “cutting” sites, diazo compounds and hypervalent iodine(III) compounds hold a critical role as versatile reagents in a wide range of organic transformations, because their excellent nucleofugal ability allows for a large number of unusual...
This article offers a materials‐chemistry perspective for colloidal quantum dots (QDs) in the field of display, including QD‐enhanced liquid‐crystal‐display (QD‐LCD) and QD‐based light‐emitting‐diodes (QLEDs) display. The rapid successes of QDs for display in the past five years are not accidental but have a deep root in both maturity of their synthetic chemistry and their unique chemical, optical, and optoelectronic properties. This article intends to discuss the natural match of QD emitters for...
Multiple bonds between boron and transition metals are known in many borylene (:BR) complexes via metal dp ® BR back donation, despite the electron‐deficiency of boron. Electron‐precise metal‐boron triple bond was first observed in BiB2O– [Bi≡B‐B≡O]–, in which both boron atoms can be viewed as being engaged in sp hybridization and the [B‐BO]– fragment is isoelectronic to a carbyne (CR). To search for the first electron‐precise transition‐metal‐boron triple bond species, we have produced IrB2O– and...
The chemical structures and topologies of the crosslinks in supramolecular networks play a crucial role in their properties and functions. Herein, we prepared a type of poly( N ‐isopropylacrylamide) (PNIPAAM)‐based supramolecular networks crosslinked by emissive hexagonal metallacycles. The topological connections in these networks greatly affect their properties, as evidenced by their differences in absorption, emission, lower critical solution temperature, and modulus along with the variation...
Magic number 28: A 28th silver atom combined with a more rigid thiolate ligand led to room‐temperature photoluminescence in radarlike silver clusters possessing similar geometrical and electronic structures (see picture). The additional silver atom triggered the emission of green light as a result of the rigidity of the cluster structure. Abstract Luminescent metal clusters show promise for applications in imaging and sensing. However, promoting emission from metal clusters at room temperature...
A 2D heterostructure of mesoporous polypyrrole grown on defective graphene oxide was used as a dual‐functional lithium ion redistributor with stepwise lithium ion distribution and homogeneous lithium deposition for extremely stable, dendrite‐free lithium anodes. This design takes advantage of the synergistic effects arising from the lithium ion transport nanochannels of mesoporous polypyrrole and the defective graphene oxide acting as a lithium ion nanosieve. Abstract Guiding the lithium ion...
Tuning on multiple channels: Multiple components of the chemical reaction network in the ATP‐driven transient DNA polymerization systems can be caged by different photocleavable groups that respond to different colors of light. As a result, light can be used to modulate the non‐equilibrium behavior and multiple wavelength‐dependent dynamic steady states. Abstract Fuel‐driven self‐assemblies are gaining ground for creating autonomous systems and materials, whose temporal behavior is preprogrammed...
Potassium salts of two pyrene‐fused azaacene diradical dianions have been isolated and fully characterized. Experimental and theoretical studies disclosed that both dianions are open‐shell singlets in the ground state and their triplet states are thermally readily accessible owing to the small singlet–triplet energy gap. Abstract Although diradicals and azaacenes have been greatly attractive in fundamental chemistry and functional materials, the isolable diradical dianions of azaacenes are...
Into the fold: Linear HVVH and folded V2(μ‐H)2 have been generated in solid Ne and were detected by infrared spectroscopy. Both molecules are characterized by multiple metal–metal bonding with a high bond order. Abstract Dinuclear compounds of early transition metals with a high metal–metal bond order are of fundamental interest due to their intriguing bonding situation and of practical interest because of their potential involvement in catalytic processes. In this work, two isomers of V2H2...
Lithium bonds that are present in lithium batteries are discussed in this Viewpoint, including historical developments, comparisons with hydrogen bonds, and their potential applications. Discourse on the chemistry of the Li bond can provide fruitful insight into the fundamental interactions within Li batteries and thus deliver a deeper understanding of their working mechanism. Abstract Lithium bonds are analogous to hydrogen bonds and are therefore expected to exhibit similar characteristics...
Precise control of assembly pathways is achieved for the self‐assembly of dipeptide molecules into aerogels with entirely different surface wettability, which resulted from charged groups or aromatic residues exposed on the surface of their nanoscale building blocks. This study paves a new way to construct single‐component supramolecular materials with different properties and functions. Abstract Constructing supramolecular materials with tunable properties and functions is a great challenge...
A novel Ni/Cu dual catalysis gives rise to fundamentally new cooperative reactivity and enables the regio‐ and enantioselective propargylic alkylation reaction. A diverse set of α‐quaternary propargylated amino ester derivatives were synthesized in good yields with excellent enantioselectivities (up to 99% ee ). This work highlights the power of cooperative catalysis, which can be expected to have broad implications in homogeneous catalysis beyond the highly valuable synthetic intermediates.
Things and R‐OHs of outrageous fortune: Easily accessible Cr complexes catalyse the alkylation of amines by alcohols in a sustainable C−N formation reaction that follows the borrowing‐hydrogen or hydrogen‐autotransfer concept. This work indicates that Cr complexes can mediate (de)hydrogenation catalysis. Abstract 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,...
Making contact: An ultra‐stable conductive Liy Sn/Li3N composite interface is formed in situ between Li6.4La3Zr1.4Ta0.6O12 (LLZTO)and Li metal by a facile conversion reaction of magnetron‐sputtered SnNx with Li metal at 300 °C for advanced all‐solid‐state high‐voltage Li metal batteries. Abstract The garnet electrolyte presents poor wettability with Li metal, resulting in an extremely large interfacial impedance and drastic growth of Li dendrites. Herein, a novel ultra‐stable conductive...
A chemical robot was designed, assembled and utilised for the discovery of supramolecular architectures through the exploration of a chemical space exceeding 109 possible reactions. By searching for reactivity differences, a range of new 1‐benzyl‐(1,2,3‐triazol‐4‐yl)‐N‐alkyl‐(2‐pyridinemethanimine) ligands were found and four new complexes of Fe and Co were discovered, autonomously discovering the rules of self‐assembly for these systems. Abstract We present a chemical discovery robot for the...
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