Metal doped core–shell Metal‐Organic Frameworks@Covalent Organic Frameworks (MOFs@COFs) are presented as a novel platform for photocatalysis. A palladium (Pd) doped MOFs@COFs in the form of ...Pd/TiATA@LZU1 shows excellent photocatalytic performance for tandem dehydrogenation and hydrogenation reactions in a continuous‐flow microreactor and a batch system, indicating the great potential of the metal doped MOFs@COFs as a multifunctional platform for photocatalysis. Explanations for the performance enhancement are elucidated. An integrated dual‐chamber microreactor coupled with the metal doped MOFs@COFs is introduced to demonstrate a concept of an intensified green photochemical process, which can be broadly extended to challenging liquid–gas tandem and cascade reactions.
Pd doped core–shell TiATA@LZU1 is fabricated and shows excellent photocatalytic performance for hydrogenation and dehydrogenation reactions in batch and in a newly designed dual‐chamber microreactor. This indicates a great promise of metal–organic frameworks@covalent organic frameworks (MOFs@COFs) hybrids as a novel platform for efficient photocatalysis.
Monoamine oxidase (MAO) is believed to mediate the degradation of monoamine neurotransmitters, including dopamine, in the brain. Between the two types of MAO, MAO-B has been believed to be involved ...in dopamine degradation, which supports the idea that the therapeutic efficacy of MAO-B inhibitors in Parkinson's disease can be attributed to an increase in extracellular dopamine concentration. However, this belief has been controversial. Here, by utilizing in vivo phasic and basal electrochemical monitoring of extracellular dopamine with fast-scan cyclic voltammetry and multiple-cyclic square wave voltammetry and ex vivo fluorescence imaging of dopamine with GRAB
, we demonstrate that MAO-A, but not MAO-B, mainly contributes to striatal dopamine degradation. In contrast, our whole-cell patch-clamp results demonstrated that MAO-B, but not MAO-A, was responsible for astrocytic GABA-mediated tonic inhibitory currents in the rat striatum. We conclude that, in contrast to the traditional belief, MAO-A and MAO-B have profoundly different roles: MAO-A regulates dopamine levels, whereas MAO-B controls tonic GABA levels.
A continuous‐flow homogeneous photocatalytic method has been devised for the direct arylation of 2H‐indazoles. This visible‐light‐promoted approach directly accesses a wide range of structurally ...diverse C3‐arylated scaffolds of biological interest in a fast (1 min), single‐step reaction by using eosin Y as an organophotocatalyst. Furthermore, a microreactor technology is also employed for the fast synthesis of liver X receptor inhibitor drugs with very good yields under metal‐free conditions, whereas the reported methods required multiple steps and much longer reaction times (18–24 h).
Lights, catalyst, action! A continuous‐flow homogeneous photocatalytic method has been devised for the direct arylation of 2H‐indazoles. This visible‐light‐promoted approach directly accesses a wide range of structurally diverse C3‐arylated scaffolds of biological interest in a fast, single‐step synthesis with eosin Y as a catalyst. A microreactor is employed for the fast synthesis of liver X receptor inhibitor drugs with very good yields.
A fierce dog: A method for the continuous in‐situ on‐demand generation, separation, and reaction of diazomethane in a dual‐channel microreactor has been developed (see picture; ...Diazald=N‐methyl‐N‐nitroso‐p‐toluenesulfonamide). The microchemical system allows a variety of diazomethane reactions to be performed without the most common problems of preparation, handling, transfer, and decomposition.
We present covalently self‐assembled peptide hollow nanocapsule and peptide lamella. These biomimetic dityrosine peptide nanostructures are synthesized by one‐step photopolymerization of a ...tyrosine‐rich short peptide without the aid of a template. This simple approach offers direct synthesis of fluorescent peptide nanocages and free‐standing thin films. The simple crosslinked peptide lamella films provide robust mechanical properties with an elastic modulus of approximately 30 GPa and a hardness of 740 MPa. These nanostructures also allow for the design of peptidosomes. The approach taken here represents a rare example of covalent self‐assembly of short peptides into nano‐objects, which may be useful as microcompartments and separation membranes.
Covalent self‐assembly of peptides: Direct synthesis of fluorescent peptide nanocapsules and free‐standing thin films by bioinspired one‐step photopolymerization of peptides is reported. The crosslinked peptides showed superior mechanical strength compared to non‐covalent peptides, and were used to design robust peptidosomes.
Self-motile Janus colloids are important for enabling a wide variety of microtechnology applications as well as for improving our understanding of the mechanisms of motion of artificial micro- and ...nanoswimmers. We present here micro/nanomotors which possess a reversed Janus structure of an internal catalytic “chemical engine”. The catalytic material (here platinum (Pt)) is embedded within the interior of the mesoporous silica (mSiO2)-based hollow particles and triggers the decomposition of H2O2 when suspended in an aqueous peroxide (H2O2) solution. The pores/gaps at the noncatalytic (Pt) hemisphere allow the exchange of chemical species in solution between the exterior and the interior of the particle. By varying the diameter of the particles, we observed size-dependent motile behavior in the form of enhanced diffusion for 500 nm particles, and self-phoretic motion, toward the nonmetallic part, for 1.5 and 3 μm ones. The direction of motion was rationalized by a theoretical model based on self-phoresis. For the 3 μm particles, a change in the morphology of the porous part is observed, which is accompanied by a change in the mechanism of propulsion via bubble nucleation and ejection as well as a change in the direction of motion.
Abstract
Tourette syndrome is a childhood-onset neuropsychiatric disorder characterized by intrusive motor and vocal tics that can lead to self-injury and deleterious mental health complications. ...While dysfunction in striatal dopamine neurotransmission has been proposed to underlie tic behaviour, evidence is scarce and inconclusive. Deep brain stimulation (DBS) of the thalamic centromedian parafascicular complex (CMPf), an approved surgical interventive treatment for medical refractory Tourette syndrome, may reduce tics by affecting striatal dopamine release. Here, we use electrophysiology, electrochemistry, optogenetics, pharmacological treatments and behavioural measurements to mechanistically examine how thalamic DBS modulates synaptic and tonic dopamine activity in the dorsomedial striatum.
Previous studies demonstrated focal disruption of GABAergic transmission in the dorsolateral striatum of rats led to repetitive motor tics recapitulating the major symptom of Tourette syndrome. We employed this model under light anaesthesia and found CMPf DBS evoked synaptic dopamine release and elevated tonic dopamine levels via striatal cholinergic interneurons while concomitantly reducing motor tic behaviour.
The improvement in tic behaviour was found to be mediated by D2 receptor activation as blocking this receptor prevented the therapeutic response. Our results demonstrate that release of striatal dopamine mediates the therapeutic effects of CMPf DBS and points to striatal dopamine dysfunction as a driver for motor tics in the pathoneurophysiology of Tourette syndrome.
Parafascicular nucleus deep brain stimulation is an effective treatment for medically refractory Tourette syndrome. Using an animal model of the disease, Rusheen et al. show that deep brain stimulation reduces motor tics via enhanced striatal dopamine activity at D2 receptors.
In a mass casualty incident, the factors that determine the survival rate of injured patients are diverse, but one of the key factors is the time for triage. Additionally, the main factor that ...determines the time of triage is the number of medical personnel. However, when relying on a small number of medical personnel, the ability to increase survivability is limited. Therefore, developing a classification model for survival prediction that can quickly and precisely triage via wearable devices without medical personnel is important. In this study, we designed a consciousness index to substitute the factor by manpower and improved the classification accuracy by applying a machine learning algorithm. First, logistic regression analysis using vital signs and a consciousness index capable of remote monitoring through wearable devices confirmed the high efficiency of the consciousness index. We then developed a classification model with high accuracy which corresponds to existing injury severity scoring systems through the machine learning algorithms. We extracted 460,865 cases which met our criteria for developing the survival prediction from the national sample project in the national trauma databank which contains 408,316 cases of blunt injury and 52,549 cases of penetrating injury. Among the dataset, 17,918 (3.9%) cases died while the other survived. The AUCs with 95% confidence intervals (CIs) for the different models with the proposed simplified consciousness score as follows: RTS (as baseline), 0.78 (95% CI = 0.775 to 0.785); logistic regression, 0.87 (95% CI = 0.862 to 0.870); random forest, 0.87 (95% CI = 0.862 to 0.872); deep neural network, 0.89 (95% CI = 0.882 to 0.890). As a result, we confirmed the possibility of remote triage using a wearable device. It is expected that the time required for triage can be effectively reduced by using the developed classification model of survival prediction.
Covalent organic frameworks (COFs) are two-dimensional/three-dimensional crystalline polymeric materials with diverse molecular backbones and topologies and are strong candidates for numerous ...applications. However, the ready availability of these materials is a challenge. The key issues are slow production rates, harsher and longer reaction conditions, and a need for post-synthetic modification to obtain desired molecular functionalities. Only a few studies, including those using microfluidic techniques, have focused on refining these factors, but these reports lack synthetic continuity and scalability. Herein, we present a fast, intensified and continuous synthesis and post-synthetic modification of β-ketoenamine-linked COFs by confining organic building units into moving microdroplets in a transparent capillary. This study introduces a one-step, facile approach to serially modify NO2 - to NH2 -substituted COFs in a fraction of the time, effort and cost of traditional methods. These results may stimulate the development of novel COFs with unique chemistries and functions for various applications.
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