High Performance Electrocatalysts Based on Pt Nanoarchitecture for Fuel Cell Applications

Fuel cells, converting chemical energy from fuels into electricity directly without the need for combustion, are promising energy conversion devices for their potential applications as environmentally friendly, energy efficient power sources. However, to take fuel cell technology forward towards commercialization, we need to achieve further improvements in electrocatalyst technology, which can play an extremely important role in essentially determining cost-effectiveness, performance, and durability. In particular, platinum- (Pt-) based electrocatalyst approaches have been extensively investigated and actively pursued to meet those demands as an ideal fuel cell catalyst due to their most outstanding activity for both cathode oxygen reduction reactions and anode fuel oxidation reactions. In this review, we will address important issues and recent progress in the development of Pt-based catalysts, their synthesis, and characterization. We will also review snapshots of research that are focused on essential dynamics aspects of electrocatalytic reactions, such as the shape effects on the catalytic activity of Pt-based nanostructures, the relationships between structural morphology of Pt-based nanostructures and electrochemical reactions on both cathode and anode electrodes, and the effects of composition and electronic structure of Pt-based catalysts on electrochemical reaction properties of fuel cells.</jats:p

Inorganic-ligand exchanging time effect in PbS quantum dot solar cell

We investigate time-dependent inorganic ligand exchanging effect and photovoltaic performance of lead sulfide (PbS) nanocrystal films. With optimal processing time, volume shrinkage induced by residual oleic acid of the PbS colloidal quantum dot (CQD) was minimized and a crack-free film was obtained with improved flatness. Furthermore, sufficient surface passivation significantly increased the packing density by replacing from long oleic acid to a short iodide molecule. It thus facilities exciton dissociation via enhanced charge carrier transport in PbS CQD films, resulting in the improved power conversion efficiency from 3.39% to 6.62%. We also found that excess iodine ions on the PbS surface rather hinder high photovoltaic performance of the CQD solar cell

Chemically encoded self-organized quantum chain supracrystals with exceptional charge and ion transport properties

Artificially grown superstructures from small building blocks is an intriguing subject in ‘bottom-up’ molecular science and nanotechnology. Although discrete nanoparticles with different morphologies and physicochemical properties are readily produced, assembly them into higher-order structure amenable to practical applications is still a considerable challenge. This report introduces a stepwise heterogeneous approach for coupling colloidal quantum dots (QDs) synthesis with self-organization to directly generate quantum chains (QCs). By using vulcanized sulfur precursors, QDs are interdigitated into microscale chainlike supracrystals associated with oleylamine and oleic acid as structure directing agents. The cooperative nature of the QD growth and assembly have been extended to fabricate binary (PbS) and ternary metal chalcogenides (CuInS2) QC superstructures over a range of length scales. In addition, enhanced ion and charge transfer performance have been demonstrated which are determined to originate from the minimum interparticle distance and nearly bare nanocrystal surface. The process reported here is general and can be readily extended to the production of many other metal chalcogenide QD superstructures for energy storage applications

Genetic and environment effects on structural neuroimaging endophenotype for bipolar disorder: a novel molecular approach

We investigated gene–environment effects on structural brain endophenotype in bipolar disorder (BD) using a novel method of combining polygenic risk scores with epigenetic signatures since traditional methods of examining the family history and trauma effects have significant limitations. The study enrolled 119 subjects, including 55 BD spectrum (BDS) subjects diagnosed with BD or major depressive disorder (MDD) with subthreshold BD symptoms and 64 non-BDS subjects comprising 32 MDD subjects without BD symptoms and 32 healthy subjects. The blood samples underwent genome-wide genotyping and methylation quantification. We derived polygenic risk score (PRS) and methylation profile score (MPS) as weighted summations of risk single nucleotide polymorphisms and methylation probes, respectively, which were considered as molecular measures of genetic and environmental risks for BD. Linear regression was used to relate PRS, MPS, and their interaction to 44 brain structure measures quantified from magnetic resonance imaging (MRI) on 47 BDS subjects, and the results were compared with those based on family history and childhood trauma. After multiplicity corrections using false discovery rate (FDR), MPS was found to be negatively associated with the volume of the medial geniculate thalamus (FDR = 0.059, partial R2 = 0.208). Family history, trauma scale, and PRS were not associated with any brain measures. PRS and MPS show significant interactions on whole putamen (FDR = 0.09, partial R2 = 0.337). No significant gene–environment interactions were identified for the family history and trauma scale. PRS and MPS generally explained greater proportions of variances of the brain measures (range of partial R2 = [0.008, 0.337]) than the clinical risk factors (range = [0.004, 0.228])

Scaling behavior of low-temperature orthorhombic domains in the prototypical high-temperature superconductor La₁.₈₇₅ Ba₀.₁₂₅ CuO₄

Structural symmetry breaking and recovery in condensed-matter systems are closely related to exotic physical properties such as superconductivity (SC), magnetism, spin density waves, and charge density waves (CDWs). The interplay between different order parameters is intricate and often subject to intense debate, as in the case of CDW order and superconductivity. In La₁.₈₇₅ Ba₀.₁₂₅ CuO

Multi-stage machine learning model for hierarchical tie valence prediction

This is the final version. Available from the Association for Computing Machinery via the DOI in this record. Data availability: Due to our non-disclosure agreement with the organization and our Institutional Review Board data management protocol, the raw data cannot be shared.Individuals interacting in organizational settings involving varying levels of formal hierarchy naturally form a complex network of social ties having different tie valences (e.g., positive and negative connections). Social ties critically affect employees' satisfaction, behaviors, cognition, and outcomes - yet identifying them solely through survey data is challenging because of the large size of some organizations or the often hidden nature of these ties and their valences. We present a novel deep learning model encompassing NLP and graph neural network techniques that identifies positive and negative ties in a hierarchical network. The proposed model uses human resource attributes as node information and web-logged work conversation data as link information. Our findings suggest that the presence of conversation data improves the tie valence classification by 8.91% compared to employing user attributes alone. This gain came from accurately distinguishing positive ties, particularly for male, non-minority, and older employee groups. We also show a substantial difference in conversation patterns for positive and negative ties with positive ties being associated with more messages exchanged on weekends, and lower use of words related to anger and sadness. These findings have broad implications for facilitating collaboration and managing conflict within organizational and other social networks.Institute for Basic Sciences (IBS), Republic of KoreaNational Research Foundation of Korea (NRF

Growth of quantum dot coated core-shell anisotropic nanowires for improved thermal and electronic transport

Anisotropic nanowires are promising candidates for electronic thermal management due to their unique electrical and thermal properties.However, eco-friendly solution-processed nanomaterials with an elaborate morphology and microstructure for modulating thermal andcharge transfer are still a considerable challenge. Herein, we present a simple but effective approach for synthesizing pseudo core-shell nano-wires through quantum dot (QD)-like nanostructure coating (p-NW@QD) to generate exceptional electron-phonon transport properties.With the assistance of diphenyl ether as a coordination solvent, high crystallinity lead sulfide NWs can be fabricated with a large aspect ratiotogether with uniform QD coating. Thisp-NW@QD exhibits high electronic mobility (30.65 cm2/Vs) as well as a diameter independent lowthermal conductivity (1.5361 W/m K). Direct charge/heat carrier flow measurements and computational simulations demonstrate that theunusual electrical and thermal transport phenomenon is strongly dependent on the fast charge transport through the QD shell, and a slowphonon migration across the Umklapp process dominated NW cores. These findings indicate a significant step toward colloidal synthesisnanostructures for future high-performance nanoelectronics and thermal energy devices

Red green blue emissive lead sulfide quantum dots: heterogeneous synthesis and applications.

Visible emission colloidal quantum dots (QDs) have shown promise in optical and optoelectronic applications. These QDs are typically composed of relatively expensive elements in the form of indium, cadmium, and gallium since alternative candidate materials exhibiting similar properties are yet to be realized. Herein, for the first time, we report red green blue (RGB) photoluminescences with quantum yields of 18% from earth-abundant lead sulfide (PbS) QDs. The visible emissive property is mainly attributed to a high degree of crystallinity even for the extremely small QD sizes (1-3 nm), which is realized by employing a heterogeneous reaction methodology at high growth temperatures (>170 °C). We demonstrate that the proposed heterogeneous synthetic method can be extended to the synthesis of other metal chalcogenide QDs, such as zinc sulfide and zinc selenide, which are promising for future industrial applications. More importantly, benefiting from the enlarged band gaps, the as-prepared PbS solar cells show an impressive open circuit voltage (∼0.8 V) beyond that reported to date

Essential and checkpoint functions of budding yeast ATM and ATR during meiotic prophase are facilitated by differential phosphorylation of a meiotic adaptor protein, Hop1

A hallmark of the conserved ATM/ATR signalling is its ability to mediate a wide range of functions utilizing only a limited number of adaptors and effector kinases. During meiosis, Tel1 and Mec1, the budding yeast ATM and ATR, respectively, rely on a meiotic adaptor protein Hop1, a 53BP1/Rad9 functional analog, and its associated kinase Mek1, a CHK2/Rad53-paralog, to mediate multiple functions: control of the formation and repair of programmed meiotic DNA double strand breaks, enforcement of inter-homolog bias, regulation of meiotic progression, and implementation of checkpoint responses. Here, we present evidence that the multi-functionality of the Tel1/Mec1-to-Hop1/Mek1 signalling depends on stepwise activation of Mek1 that is mediated by Tel1/Mec1 phosphorylation of two specific residues within Hop1: phosphorylation at the threonine 318 (T318) ensures the transient basal level Mek1 activation required for viable spore formation during unperturbed meiosis. Phosphorylation at the serine 298 (S298) promotes stable Hop1-Mek1 interaction on chromosomes following the initial phospho-T318 mediated Mek1 recruitment. In the absence of Dmc1, the phospho-S298 also promotes Mek1 hyper-activation necessary for implementing meiotic checkpoint arrest. Taking these observations together, we propose that the Hop1 phospho-T318 and phospho-S298 constitute key components of the Tel1/Mec1- based meiotic recombination surveillance (MRS) network and facilitate effective coupling of meiotic recombination and progression during both unperturbed and challenged meiosis

Consecutive junction-induced efficient charge separation mechanisms for high-performance MoS2/quantum dot phototransistors

Phototransistors that are based on a hybrid vertical heterojunction structure of two-dimensional (2D)/quantum dots (QDs) have recently attracted attention as a promising device architecture for enhancing the quantum efficiency of photodetectors. However, to optimize the device structure to allow for more efficient charge separation and transfer to the electrodes, a better understanding of the photophysical mechanisms that take place in these architectures is required. Here, we employ a novel concept involving the modulation of the built-in potential within the QD layers for creating a new hybrid MoS2/PbS QDs phototransistor with consecutive type II junctions. The effects of the built-in potential across the depletion region near the type II junction interface in the QD layers are found to improve the photoresponse as well as decrease the response times to 950 μs, which is the faster response time (by orders of magnitude) than that recorded for previously reported 2D/QD phototransistors. Also, by implementing an electric-field modulation of the MoS2 channel, our experimental results reveal that the detectivity can be as large as 1 × 1011 jones. This work demonstrates an important pathway toward designing hybrid phototransistors and mixed-dimensional van der Waals heterostructures