| 1. |
- Han, Jingrui, et al.
(author)
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Lattice Oxygen Activation through Deep Oxidation of Co4N by Jahn–Teller–Active Dopants for Improved Electrocatalytic Oxygen Evolution
- 2024
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In: Angewandte Chemie International Edition. - : John Wiley & Sons. - 1433-7851 .- 1521-3773. ; 63:33
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Journal article (peer-reviewed)abstract
- Triggering the lattice oxygen oxidation mechanism is crucial for improving oxygen evolution reaction (OER) performance, because it could bypass the scaling relation limitation associated with the conventional adsorbate evolution mechanism through the direct formation of oxygen–oxygen bond. High-valence transition metal sites are favorable for activating the lattice oxygen, but the deep oxidation of pre-catalysts suffers from a high thermodynamic barrier. Here, taking advantage of the Jahn–Teller (J–T) distortion induced structural instability, we incorporate high-spin Mn3+ ( ) dopant into Co4N. Mn dopants enable a surface structural transformation from Co4N to CoOOH, and finally to CoO2, as observed by various in situ spectroscopic investigations. Furthermore, the reconstructed surface on Mn-doped Co4N triggers the lattice oxygen activation, as evidenced experimentally by pH-dependent OER, tetramethylammonium cation adsorption and online electrochemical mass spectrometry measurements of 18O-labelled catalysts. In general, this work not only offers the introducing J–T effect approach to regulate the structural transition, but also provides an understanding about the influence of the catalyst's electronic configuration on determining the reaction route, which may inspire the design of more efficient catalysts with activated lattice oxygen.
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| 2. |
- Han, Mei, et al.
(author)
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Promoted Self-construction of β-NiOOH in Amorphous High Entropy Electrocatalysts for the Oxygen Evolution Reaction
- 2022
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In: Applied Catalysis B. - : Elsevier. - 0926-3373 .- 1873-3883. ; 301
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Journal article (peer-reviewed)abstract
- The exploration of an efficient electrocatalyst for the oxygen evolution reaction (OER) is urgently required for sustainable renewable-energy conversion and storage. Due to the increased chemical complexity, multimetallic catalysts provide flexibility to alter their electronic and crystal structure to attain a superior intrinsic catalytic activity via synergistic effects, which is seldom accomplished using single metal catalysts. However, the high chemical complexity increases the difficulty to prepare elemental homogenous catalysts and reveal their synergistic effect during OER process, which further hinder the design of multimetallic catalysts. Here, high entropy concept is utilized to design an NiFeCoMnAl oxide with amorphous structure as OER catalyst. The direct evidence of active Ni sites is provided by the operando Raman measurements and Fe can modify oxygen intermediates binding energy on Ni sites. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) reveal that the incorporation of Mn can construct the electron-rich environment of active Ni center, and the relatively lower oxidation state of Ni facilitates the self-construction of β-NiOOH intermediates, which shows promoted OER activity as confirmed by density functional theory calculations. Doping Co can enhance the conductivity and doping Al leads to the formation of nanoporous structure through dealloying process, thus each component is essential for improving OER performance. The optimized NiFeCoMnAl catalyst exhibits an overpotential of 190 mV at 10 mA cm-2 in 1 M KOH solution, much superior to the ternary and quaternary counterparts. This work sheds light on understanding the origin of high entropy catalysts’ OER activity and thereby enables the rational design of multinary transition metallic catalysts.
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| 3. |
- Huang, Yingzhou, et al.
(author)
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Surfactant-Promoted Reductive Synthesis of Shape-Controlled Gold Nanostructures
- 2009
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In: Crystal Growth & Design. - : American Chemical Society (ACS). - 1528-7483 .- 1528-7505. ; 9:2, s. 858-862
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Journal article (peer-reviewed)abstract
- We describe a surfactant-promoted reductive route for the shape-controlled synthesis of gold nanostructures by hydrothermal treatment of chloroauric acid in the presence of the surfactant hexadecyltrimethylammonium bromide (CTAB) without using reducing agent. The results show that the cationic surfactant CTAB provides the dual function of promoting Au-III reduction to Au-0 and size- and shape-controlled synthesis of the gold nanocrystals. More importantly, the benefit of the present work stems from the first report on the controlled synthesis of gold nanostructures by hydrothermal treatment of chloroauric acid in the presence of the surfactant CTAB without using reducing agent. The kinetics of the reduction could be manipulated through changes in the CTAB concentration to produce gold nanostructures with shapes ranging from three-dimensional (313) octahedra, triangles, to two-dimensional (213) hexagonal nanoplates in high yields. Growth of gold nanostructures in the CTAB solution with concentration was monitored by microscopic and spectroscopic techniques.
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| 4. |
- Ji, Linong, et al.
(author)
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ISIS 449884 Injection Add-On to Metformin in Patients with Type 2 Diabetes: A Randomized, Double-Blind, Placebo-Controlled, Phase II Clinical Study
- 2024
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In: DIABETES THERAPY. - 1869-6953 .- 1869-6961.
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Journal article (peer-reviewed)abstract
- Introduction: ISIS 449884, a 2 '-O-methoxyethyl antisense oligonucleotide that targets the glucagon receptor (GCGR), has demonstrated an ability to reduce hepatic glucose output and lower the blood glucose level. The primary objective of this study was to investigate the safety and efficacy of ISIS 449884 as an add-on to metformin in a population of Chinese patients with type 2 diabetes mellitus (T2DM). Method: This was a multicenter, placebo-controlled (2:1), randomized, double-blind, parallel-enrollment, multiple-dose phase II study in Chinese patients with T2DM. A total of 90 patients who were uncontrolled by stable metformin monotherapy were randomized into three cohorts. Thirty subjects were enrolled in each cohort and received injections of ISIS 449884 (50 mg or 60 mg weekly or 100 mg every other week) or a corresponding volume of placebo (0.25 mL and 0.3 mL weekly or 0.5 mL every other week) subcutaneously in a 2:1 ratio for 16 weeks. Results: The primary efficacy endpoint was analyzed in 88 subjects (ISIS 449884, n = 59; placebo, n = 29). The corrected LS mean change from baseline in glycated hemoglobin (HbA1c) at week 17 in the pooled ISIS 449884 treatment group was - 1.31% (95% CI - 1.66%, - 0.96%), and that in the pooled placebo group was 0.15% (95% CI - 0.37%, 0.66%). The LS mean difference between the two groups was - 1.46% (95% CI - 1.92%, - 1.00%, P < 0.001). Treatment-emergent adverse events (TEAEs) occurred in 53/60 subjects (88.3%) and 25/30 subjects (83.3%) in the pooled ISIS 449884 treatment group and the pooled placebo group, respectively, with similar incidences. Drug-related TEAEs occurred in 41/60 subjects (68.3%) and 9/30 subjects (30.0%), respectively. TEAEs of grade 3 or higher occurred in 5/60 (8.3%) subjects and 2/30 (6.7%) subjects, respectively, and none of them were drug related. Conclusions: The ISIS 449884 injection add-on to metformin significantly reduced HbA1c in patients with T2DM uncontrolled by stable metformin monotherapy and showed an acceptable benefit/risk profile.
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| 5. |
- Kanoni, Stavroula, et al.
(author)
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Implicating genes, pleiotropy, and sexual dimorphism at blood lipid loci through multi-ancestry meta-analysis.
- 2022
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In: Genome biology. - : Springer Science and Business Media LLC. - 1474-760X .- 1465-6906 .- 1474-7596. ; 23:1
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Journal article (peer-reviewed)abstract
- Genetic variants within nearly 1000 loci are known to contribute to modulation of blood lipid levels. However, the biological pathways underlying these associations are frequently unknown, limiting understanding of these findings and hindering downstream translational efforts such as drug target discovery.To expand our understanding of the underlying biological pathways and mechanisms controlling blood lipid levels, we leverage a large multi-ancestry meta-analysis (N=1,654,960) of blood lipids to prioritize putative causal genes for 2286 lipid associations using six gene prediction approaches. Using phenome-wide association (PheWAS) scans, we identify relationships of genetically predicted lipid levels to other diseases and conditions. We confirm known pleiotropic associations with cardiovascular phenotypes and determine novel associations, notably with cholelithiasis risk. We perform sex-stratified GWAS meta-analysis of lipid levels and show that 3-5% of autosomal lipid-associated loci demonstrate sex-biased effects. Finally, we report 21 novel lipid loci identified on the X chromosome. Many of the sex-biased autosomal and X chromosome lipid loci show pleiotropic associations with sex hormones, emphasizing the role of hormone regulation in lipid metabolism.Taken together, our findings provide insights into the biological mechanisms through which associated variants lead to altered lipid levels and potentially cardiovascular disease risk.
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| 6. |
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| 7. |
- Liang, Hongyan, et al.
(author)
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Controlled Synthesis of Uniform Silver Nanospheres
- 2010
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In: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 114:16, s. 7427-7431
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Journal article (peer-reviewed)abstract
- We describe a new route, in which the polyethylene glycol (PEG) is used both as a solvent and reducing reagent and the polymer polyvinglpyrrolidone (PVP) is used as capping agent, for the synthesis of monodisperse silver nanoparticles. Uniform nanospheres with an average diameter of 54 nm can be routinely synthesized in high yield through this approach by using a PVP/AgNO3 molar ratio of 8 at 260 degrees C. Both the reaction temperature and the PVP/AgNO3 molar ratio are crucial for the diameters and size distributions of the nanospheres.
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| 8. |
- Liang, Hongyan, et al.
(author)
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High-Yield Uniform Synthesis and Microstructure-Determination of Rice-Shaped Silver Nanocrystals
- 2009
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 1520-5126 .- 0002-7863. ; 131:17, s. 6068-6068
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Journal article (peer-reviewed)abstract
- High-yield uniform silver nanorices were synthesized by a facile polyol process without the introduction of shape-selected seeds. Nanorices exhibit two plasmon resonance peaks in the visible and near-infrared regions respectively due to their anisotropy. XRD patterns demonstrated the HCP phase coexists with the FCC phase in nanorices. The novel structure of nanorices was characterized by TEM study which shows that the intergrowth of FCC and a small amount of HCP phase, nanoscale FCC (111) twinning structure, and multimodulated structures formed by a complicated stacking sequence along the long axis direction. The correlation between morphology and microstructure is discussed.
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| 9. |
- Liang, Hongyan, et al.
(author)
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Silver Nanorice Structures: Oriented Attachment-Dominated Growth, High Environmental Sensitivity, and Real-Space Visualization of Multipolar Resonances
- 2012
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In: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 24:12, s. 2339-2346
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Journal article (peer-reviewed)abstract
- We have synthesized and investigated the anisotropic growth of interesting silver nanorice. Its growth is kinetically controlled at 100 degrees C, and both oriented attachment and Ostwald ripening are involved, with the former growth mode dominating the anisotropic growth of the nanorice along the < 111 > direction. This one-directional growth is initiated by an indispensable seed-selection process, in which oxygen plays a critical role in oxidatively etching twinned silver crystals. The inhibition of this process by removing oxygen essentially blocks the nanorice growth. Although increasing reaction temperature to 120 degrees C accelerates the one-dimensional growth along the < 111 > direction, further temperature increase to 160 degrees C makes the oriented attachment dominated one-directional growth disappear; instead, the diffusion-controlled two-dimensional growth leads to the emergence of highly faceted truncated triangular and hexagonal plates mainly bound by low energy faces of {111}. Interestingly, we also found that the longitudinal surface plasmon resonance of the nanorice structures is highly sensitive to the refractive index of surrounding dielectric media, which predicts their promising applications as chemical or biological sensors. Moreover, the multipolar plasmonic resonances in these individual nanorice structures are visualized in real space, using high-resolution electron energy-loss spectroscopy.
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| 10. |
- Ma, Jiantao, et al.
(author)
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A Peripheral Blood DNA Methylation Signature of Hepatic Fat Reveals a Potential Causal Pathway for Nonalcoholic Fatty Liver Disease
- 2019
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In: Diabetes. - : AMER DIABETES ASSOC. - 0012-1797 .- 1939-327X. ; 68:5, s. 1073-1083
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Journal article (peer-reviewed)abstract
- Nonalcoholic fatty liver disease (NAFLD) is a risk factor for type 2 diabetes (T2D). We aimed to identify the peripheral blood DNA methylation signature of hepatic fat. We conducted epigenome-wide association studies of hepatic fat in 3,400 European ancestry (EA) participants and in 401 Hispanic ancestry and 724 African ancestry participants from four population-based cohort studies. Hepatic fat was measured using computed tomography or ultrasound imaging and DNA methylation was assessed at >400,000 cytosine-guanine dinucleotides (CpGs) in whole blood or CD14+ monocytes using a commercial array. We identified 22 CpGs associated with hepatic fat in EA participants at a false discovery rate <0.05 (corresponding P = 6.9 x 10(-6)) with replication at Bonferroni-corrected P < 8.6 x 10(-4). Mendelian randomization analyses supported the association of hypomethylation of cg08309687 (LINC00649) with NAFLD (P = 2.5 x 10(-4)). Hypomethylation of the same CpG was also associated with risk for new-onset T2D (P = 0.005). Our study demonstrates that a peripheral blood-derived DNA methylation signature is robustly associated with hepatic fat accumulation. The hepatic fat-associated CpGs may represent attractive biomarkers for T2D. Future studies are warranted to explore mechanisms and to examine DNA methylation signatures of NAFLD across racial/ethnic groups.
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