Alloys of transition-metal dichalcogenide can display distinctive phase evolution because of their two-dimensional structures. Herein, we report the colloidal synthesis of Mo1–x V x Se2 alloy nanosheets with full composition tuning. Alloying led to a phase transition at x = 0.7 from the semiconducting 2H phase MoSe2 to the metallic 1T phase VSe2. It also produced significant V and Se vacancies, which became the richest in the 2H phase at x = 0.3–0.5. Extensive spin-polarized density functional theory calculations consistently predicted the 2H–1T phase transition at x = 0.7, in agreement with the experimental results. The vacancy formation energy also supports the formation of V and Se vacancies. Alloying in the 2H phase enhanced the electrocatalytic performance toward hydrogen evolution reaction (HER) at x = 0.3 (in 0.5 M H2SO4) or 0.4 (in 1 M KOH). The Gibbs free energy along the HER pathway indicates that this maximum performance is due to the highest concentration of active V and Se vacancy sites.
Earth-abundant transition metal dichalcogenide nanosheets have emerged as an excellent catalyst for electrochemical water splitting to generate H2. Alloying the nanosheets with heteroatoms is a promising strategy to enhance their catalytic performance. Herein, we synthesized hexagonal (2H) phase Mo1–x Nb x Se2 nanosheets over the whole composition range using a solvothermal reaction. Alloying results in a variety of atomic-scale crystal defects such as Se vacancies, metal vacancies, and adatoms. The defect content is maximized when x approaches 0.5. Detailed structure analysis revealed that the NbSe2 bonding structures in the alloy phase are more disordered than the MoSe2 ones. Compared to MoSe2 and NbSe2, Mo0.5Nb0.5Se2 exhibits much higher electrocatalytic performance for hydrogen evolution reaction. First-principles calculation was performed for the formation energy in the models for vacancies and adatoms, supporting that the alloy phase has more defects than either NbSe2 or MoSe2. The calculation predicted that the separated NbSe2 domain at x = 0.5 favors the concurrent formation of Nb/Se vacancies and adatoms in a highly cooperative way. Moreover, the Gibbs free energy along the reaction path suggests that the enhanced HER performance of alloy nanosheets originates from the higher concentration of defects that favor H atom adsorption.
c Four different rapid diagnostic tests (RDTs) for malaria were evaluated by testing 82 healthy control patients, 89 Plasmodium vivax-infected patients, and 92 rheumatoid factor (RF)-positive nonmalaria patients. The false-positive rate ranged from 2.2% to 13% in RF-positive patients. High RF levels are associated with malaria RDT false positivity. M alaria remains a major global health problem in tropical and subtropical countries, with high morbidity and mortality and extensive economic loss (1). Malaria rapid diagnostic tests (RDTs) are becoming the clinical diagnostic method of choice due to their quick results and ease of use, even by inexperienced personnel (2). However, false-positive results may be observed in patients with rheumatoid factor (RF), hepatitis C, toxoplasmosis, human African trypanosomiasis, dengue, leishmaniasis, Chagas disease, and schistosomiasis (2). Iqbal et al. (3) reported that 33 of the 35 false-positive specimens were negative when the RF was absorbed in the immunochromatographic test (ICT). The goal of this study was to use four different malaria RDTs to explore the relationship between false-positive malaria RDT results and RF.Between April 2010 and August 2013, a total of 263 wholeblood samples with EDTA were collected from South Korean patients at the Korea University Guro Hospital, Republic of Korea. Of these 263 samples, 89 were infected with malaria, as confirmed by Giemsa-stained microscopic examination, 92 did not have malaria but did have RF, and 82 had neither malaria nor RF. Both microscopy and PCR were used to rule out malaria. Each patient provided informed consent under the protocol for human use, which was approved by the Human Use Ethical Committee, Korea University Guro Hospital.Thick and thin blood films were prepared when blood was drawn in accordance with standard procedures. These films were stained with Giemsa and examined by trained microscopists who did not have prior knowledge of the patients' clinical history. Plasmodium species and the parasite density were determined. The circumsporozoite protein (CSP) gene of Plasmodium vivax was amplified by PCR using previously established methods (4). Four commercial malaria RDT kits were selected based on the multiple target antigens (Ags) detected, the BinaxNOW malaria kit (Binax Inc., Scarborough, ME, USA), the OptiMAL-IT malaria kit (BioRad, Marnes la Coquette, France), the SD Bioline malaria Ag Pf/ Pan rapid test (Standard Diagnostics, Inc., Yongin, South Korea), and the Humasis malaria P.f/Pan antigen test (Humasis, Anyang, South Korea). BinaxNOW detects both histidine-rich protein 2 (HRP-2), which is specific to Plasmodium falciparum, and aldolase, which is a pan-malarial enzyme found in the five human pathogenic Plasmodium species (5). OptiMAL-IT differentiates P. falciparum-specific lactate dehydrogenase (PfLDH) and pan-Plasmodium lactate dehydrogenase (pLDH) by immunological detection (6). The SD Bioline and Humasis tests target HRP-2 for P. falciparum and pLDH for other human malaria species (7,8). All te...
Tissue engineering has significantly contributed to the development of optimal treatments for individual injury sites based on their unique functional and histologic properties. Human organs and tissue have three-dimensional (3D) morphologies; for example, the morphology of the eye is a spherical shape. However, most conventional electrospinning equipment is only capable of fabricating a two-dimensional (2D) structured fibrous scaffold and no report is available on a 3D electrospinning method to fabricate a hemispherical scaffold to mimic the native properties of the cornea, including microscopic to macroscopic morphology and transparency. We proposed a novel electrospinning method using a single nonconductive hemispherical device and a metal pin. A designed peg-top shaped collector, a hemispherical nonconductive device with a metal pin in the center and copper wire forming a circle around at the edge was attached to a conventional conductive collector. A 3D hemispherical transparent scaffold with radially aligned nanofibers was successfully fabricated with the designed peg-top collector. In summary, our fabricated 3D electrospun scaffold is expected to be suitable for the treatment of injuries of ocular tissues owing to the hemispherical shape and radially aligned nanofibers which can guide the direction of the main collagen and cellular actin filament in the extracellular matrix.
Polytypes of two-dimensional transition metal dichalcogenide can extend the architecture and application of nanostructures. Herein, Nb1–x V x Se2 alloy nanosheets in the full composition range (x) were synthesized by a colloidal reaction. At x = 0.1–0.3, a phase transition occurred from various hexagonal (three 2H and one 4H types) phase NbSe2 to an atomically homogeneous 1T phase VSe2. Density functional theory calculations also revealed a polytypic phase transition at x = 0.3, which was shifted close to 0 in the presence of Se vacancies. Furthermore, the calculations validate favorable formation of Se vacancies at the phase transition. The sample at x = 0.3 exhibited enhanced electrocatalytic activity toward the hydrogen evolution reaction (HER) in 0.5 M H2SO4. The Gibbs free energy indicates that the catalytic HER performance is correlated with the active Se vacancy sites of polytypic structures.
Tuning the electronic structures of transition metal dichalcogenides (TMD) is essential for their implementation in next-generation energy technologies. In this study, we synthesized composition-tuned WSe2–VSe2 (W1–x V x Se2, x = 0–1) alloyed nanosheets using a colloidal reaction. Alloying the semiconducting WSe2 with VSe2 converts the material into a metallic one, followed by a 2H-to-1T phase transition at x = 0.7. Over a wide composition range, WSe2 and VSe2 are atomically immiscible and form separate ordered domains. The miscible alloy at x = 0.1 displayed enhanced electrocatalytic activity toward the hydrogen evolution reaction (HER) in an acidic electrolyte. This trend was correlated with the d-band center via a volcano-type relationship. Spin-polarized density functional theory calculations consistently predicted the atomic immiscibility, which became more significant at the 2H-1T phase transition composition. The Gibbs free energy of H adsorption on the basal planes (Se or hole sites) and the activation barriers along the Volmer–Heyrovsky reaction pathway supported the enhanced HER performance of the alloy phase, suggesting that the dispersed V-doped structures were responsible for the best HER catalytic activity. Our study demonstrates how the atomic structure of TMD alloy nanosheets plays a crucial role in enhancing catalytic activity.
Aspergillus fumigatus is an opportunistic fungal pathogen for immunocompromised patients, and genes involved in siderophore metabolism have been identified as virulence factors. Recently, we identified the membrane transporters sit1 and sit2, which are putative virulence factors of A. fumigatus; sit1 and sit2 are homologous to yeast Sit1, and sit1 and sit2 gene expression was up-regulated after iron depletion. When expressed heterologously in Saccharomyces cerevisiae, sit1 and sit2 were localized to the plasma membrane; sit1 efficiently complemented ferrichrome (FC) and ferrioxamine B (FOB) uptake in yeast cells, whereas sit2 complemented only FC uptake. Deletion of sit1 resulted in a decrease in FOB and FC uptake, and deletion of sit2 resulted in a decrease in FC uptake in A. fumigatus It is of interest that a sit1 and sit2 double-deletion mutant resulted in a synergistic decrease in FC uptake activity. Both sit1 and sit2 were localized to the plasma membrane in A. fumigatus The expression levels of the sit1 and sit2 genes were dependent on hapX under low-but not high-iron conditions. Furthermore, mirB, and sidA gene expression was up-regulated and sreA expression down-regulated when sit1 and sit2 were deleted. Although sit1 and sit2 failed to affect mouse survival rate, these genes affected conidial killing activity. Taken together, our results suggest that sit1 and sit2 are siderophore transporters and putative virulence factors localized to the plasma membrane.
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