The electrochemical N2 fixation, which is far from practical application in aqueous solution under ambient conditions, is extremely challenging and requires a rational design of electrocatalytic ...centers. We observed that bismuth (Bi) might be a promising candidate for this task because of its weak binding with H adatoms, which increases the selectivity and production rate. Furthermore, we successfully synthesized defect‐rich Bi nanoplates as an efficient noble‐metal‐free N2 reduction electrocatalyst via a low‐temperature plasma bombardment approach. When exclusively using 1H NMR measurements with N2 gas as a quantitative testing method, the defect‐rich Bi(110) nanoplates achieved a 15NH3 production rate of 5.453 μg mgBi−1 h−1 and a Faradaic efficiency of 11.68 % at −0.6 V vs. RHE in aqueous solution at ambient conditions.
Beneficial defects: Defect‐rich bismuth nanoplates achieve a 15NH3 production rate of 5.453 μg mgBi−1 h−1 and a Faradaic efficiency of 11.68 % at −0.6 V vs. RHE in aqueous solutions at ambient conditions because of their poor binding with H adatoms, which increases the selectivity and production rate. Also, 1H NMR measurements with N2 gas ware used as a quantitative test method in aqueous electrolytes.
Major depressive disorder (MDD) is common and disabling, but its neuropathophysiology remains unclear. Most studies of functional brain networks in MDD have had limited statistical power and data ...analysis approaches have varied widely. The REST-meta-MDD Project of resting-state fMRI (R-fMRI) addresses these issues. Twenty-five research groups in China established the REST-meta-MDD Consortium by contributing R-fMRI data from 1,300 patients with MDD and 1,128 normal controls (NCs). Data were preprocessed locally with a standardized protocol before aggregated group analyses. We focused on functional connectivity (FC) within the default mode network (DMN), frequently reported to be increased in MDD. Instead, we found decreased DMN FC when we compared 848 patients with MDD to 794 NCs from 17 sites after data exclusion. We found FC reduction only in recurrent MDD, not in first-episode drug-naïve MDD. Decreased DMN FC was associated with medication usage but not with MDD duration. DMN FC was also positively related to symptom severity but only in recurrent MDD. Exploratory analyses also revealed alterations in FC of visual, sensory-motor, and dorsal attention networks in MDD. We confirmed the key role of DMN in MDD but found reduced rather than increased FC within the DMN. Future studies should test whether decreased DMN FC mediates response to treatment. All R-fMRI indices of data contributed by the REST-meta-MDD consortium are being shared publicly via the R-fMRI Maps Project.
Alcoholic liver disease (ALD) remains an important health problem worldwide. Perturbation of micronutrients has been broadly reported to be a common characteristic in patients with ALD, given the ...fact that micronutrients often act as composition or coenzymes of many biochemical enzymes responsible for the inflammatory response, oxidative stress, and cell proliferation. Mapping the metabolic pattern and the function of these micronutrients is a prerequisite before targeted intervention can be delivered in clinical practice. Recent years have registered a significant improvement in our understanding of the role of micronutrients on the pathogenesis and progression of ALD. However, how and to what extent these micronutrients are involved in the pathophysiology of ALD remains largely unknown. In the current study, we provide a review of recent studies that investigated the imbalance of micronutrients in patients with ALD with a focus on zinc, iron, copper, magnesium, selenium, vitamin D and vitamin E, and determine how disturbances in micronutrients relates to the pathophysiology of ALD. Overall, zinc, selenium, vitamin D, and vitamin E uniformly exhibited a deficiency, and iron demonstrated an elevated trend. While for copper, both an elevation and deficiency were observed from existing literature. More importantly, we also highlight several challenges in terms of low sample size, study design discrepancies, sample heterogeneity across studies, and the use of machine learning approaches.
The tuning of metal–organic framework (MOF) nanosheet stacking modes from molecular level was rarely explored although it significantly affected the properties and applications of nanosheets. Here, ...the different stacking modes of Zr‐1, 3, 5‐(4‐carboxylphenyl)‐benzene framework nanosheets were synthesized through the induction of different host–guest noncovalent interactions. The solvents of methyl benzene and ethyl acetate induced twisted stacking of nanosheets with the specific rotation angles of 12°, 18°, 24° and 6°, 18°, 24°, 30°, respectively, which was in agreement with theoretical calculations. Meanwhile, the alkanes were likely to vertically enter the pores of Zr‐BTB nanosheets because of steric hindrance and hydrophobic interactions, resulting in the untwisted stacking of nanosheets. The untwisted ordered nanopores showed the excellent gas chromatographic separations of benzene derivative isomers, which was better than twisted nanosheets stacking and commercial columns. This work uncovers a rational strategy to control the stacking of two‐dimensional MOF nanosheets.
The host–guest noncovalent strategy was proposed to tune the stacking modes of metal–organic framework nanosheets for isomer separation. Solvents of methyl benzene and ethyl acetate induced twisted stacking of nanosheets, while the alkanes from C6 to C14 were likely to vertically enter the pores of nanosheets, resulting in the untwisted stacking of nanosheets as efficient isomer separator.
Aberrant topological organization of whole-brain networks has been inconsistently reported in studies of patients with major depressive disorder (MDD), reflecting limited sample sizes. To address ...this issue, we utilized a big data sample of MDD patients from the REST-meta-MDD Project, including 821 MDD patients and 765 normal controls (NCs) from 16 sites. Using the Dosenbach 160 node atlas, we examined whole-brain functional networks and extracted topological features (e.g., global and local efficiency, nodal efficiency, and degree) using graph theory-based methods. Linear mixed-effect models were used for group comparisons to control for site variability; robustness of results was confirmed (e.g., multiple topological parameters, different node definitions, and several head motion control strategies were applied). We found decreased global and local efficiency in patients with MDD compared to NCs. At the nodal level, patients with MDD were characterized by decreased nodal degrees in the somatomotor network (SMN), dorsal attention network (DAN) and visual network (VN) and decreased nodal efficiency in the default mode network (DMN), SMN, DAN, and VN. These topological differences were mostly driven by recurrent MDD patients, rather than first-episode drug naive (FEDN) patients with MDD. In this highly powered multisite study, we observed disrupted topological architecture of functional brain networks in MDD, suggesting both locally and globally decreased efficiency in brain networks.
Precise shaping of metal–organic frameworks (MOFs) is significant in both fundamental coordination chemistry and practical applications, such as catalysis, separation, and biomedicine. Herein, we ...demonstrated a linker scissoring strategy for precisely shaping MOFs through surface conformational pairing. In this strategy, the bidentate linkers which were designed according to the original tetratopic ligands and the coordination environment of MOF surfaces, were utilized as the covering agents. The shape of these covering agents and the surface conformation of metals onto MOFs restricted them to coordinate on specific MOF facets thus precisely controlling the shape of the MOFs. Different shapes of PCN‐608 from nanoplate (PCN‐NP) to nanorod (PCN‐NR) have been targeted by adding different bidentate linkers. The universality of this strategy was demonstrated by controlling the shapes of the NU‐MOFs from nanoplate to nanorod. This strategy provides a new guiding principle to synthesize MOF nanocrystals with controlled shapes.
A “linker scissoring” strategy is used to control the shape of metal–organic framework (MOF) nanoparticles from nanoplate to nanorod by surface conformational pairing. Both structure and shape influenced the separation ability of MOF stationary phases in gas chromatography by affecting the thermodynamic and kinetic diffusion factors.
Identification of rapid, inexpensive, and reliable prognostic factors can improve survival estimation and guide healthcare in patients with acute heart failure (AHF). In this study, we aimed to ...determine the prognostic value of the platelet-to-lymphocyte ratio (PLR) in patients with AHF. A total of 443 patients from two hospitals met the inclusion criteria from January 2010 to December 2017. Univariate and multivariate Cox analyses were performed to determine the association of PLR with survival. All-cause mortality was analysed using the Kaplan-Meier method. The 6-month survival rate for patients according to PLR quartiles (<110.63, 110.63-139.23, 139.23-177.17, and >177.17) were 90.09%, 76.79%, 50.07%, and 37.27%, respectively (p < 0.001). Univariate analysis identified high PLR (>110.63), old age (≥73 years), smoking habit, low estimated glomerular filtration rate (<57), and high platelet count (≥198 × 10
/l) as poor prognostic factors for survival. In the multivariate analysis, after adjusting for confounding factors, the third (hazard ratio HR = 3.118, 95% confidence interval CI = 1.668-5.386, p < 0.001) and fourth (HR = 2.437, 95% CI = 1.302-3.653, p < 0.001) quartiles of PLR were identified as independent prognostic factors in patients with AHF. A higher PLR was associated with poor clinical outcomes in patients with AHF and might be a novel marker in AHF management.
Ligand‐induced surface restructuring with heteroatomic doping is used to precisely modify the surface of a prototypical Au25(SR1)18− cluster (1) while maintaining its icosahedral Au13 core for the ...synthesis of a new bimetallic Au19Cd3(SR2)18− cluster (2). Single‐crystal X‐ray diffraction studies reveal that six bidentate Au2(SR1)3 motifs (L2) attached to the Au13 core of 1 were replaced by three quadridentate Au2Cd(SR2)6 motifs (L4) to create a bimetallic cluster 2. Experimental and theoretical results demonstrate a stronger electronic interaction between the surface motifs (Au2Cd(SR2)6) and the Au13 core, attributed to a more compact cluster structure and a larger energy gap of 2 compared to that of 1. These factors dramatically enhance the photoluminescence quantum efficiency and lifetime of crystal of the cluster 2. This work provides a new route for the design of a wide range of bimetallic/alloy metal nanoclusters with superior optoelectronic properties and functionality.
On the surface of it: Ligand‐induced surface restructuring with heteroatomic doping is used to precisely modify the surface of a prototypical Au25(SR1)18− cluster while maintaining its icosahedral Au13 core for the synthesis of a new bimetallic Au19Cd3(SR2)18− cluster.
Alcoholic liver disease (ALD) is characterized by hepatocyte damage, inflammatory cell activation, and increased intestinal permeability leading to the clinical manifestations of alcoholic hepatitis. ...Selected members of the family of microRNAs (miRNAs) are affected by alcohol, resulting in an abnormal miRNA profile in the liver and circulation in ALD. Increasing evidence suggests that miRNAs that regulate inflammation, lipid metabolism and promote cancer are affected by excessive alcohol administration in mouse models of ALD. This communication highlights recent findings in miRNA expression and functions as they relate to the pathogenesis of ALD. The cell‐specific distribution of miRNAs, as well as the significance of circulating extracellular miRNAs, is discussed as potential biomarkers. Finally, the prospects of miRNA‐based therapies are evaluated in ALD.
Highlights
The targets of microRNAs (miRNAs) in alcoholic liver disease (ALD).
The regulation roles of miRNAs in ALD.
Potential clinical application of miRNAs as diagnostic markers in ALD.
The future application prospect of miRNAs in ALD.
This review highlights recent findings in microRNAs (miRNA) expression and functions as they relate to the pathogenesis of alcoholic liver disease (ALD). The cell‐specific distribution of miRNAs, as well as the significance of circulating extracellular miRNAs, is discussed as potential biomarkers. Finally, the prospects of miRNA‐based therapies are evaluated in ALD.
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