Latest ArticlesHydrogen energy could be a economic and powerful technology for sustainable future. Producing hydrogen fuel by electrochemical water splitting has attracted intense interest. Due to their physical and chemical properties, two-dimensional (2D) nanomaterials have sparked immense interest in water electrocatalysis for hydrogen production. This review focuses on the emerging nanocatalysts in 2D nanoarchitectures for electrocatalytic hydrogen production. The fundamentals of HER are firstly depicted, following the discussion of recent advances in typical 2D electrocatalysts for HER. The insights into the relationship among the synthetic protocols, structure, catalytic performance and thermodynamics will be discussed in details. Finally, the outlooks regarding further development of 2D nanocatalysts for HER are proposed. We hope this review will offer a comprehensive understanding in 2D nanocatalysts to promote electrochemical hydrogen production.
The rapid detection of microparticles exhibits a broad range of applications in the field of science and technology. The proposed method differentiates and identifies the 2 µm and 5 µm sized particles using a laser light scattering. The detection method is based on measuring forward light scattering from the particles and then classifying the acquired data using support vector machines. The device is composed of a microfluidic chip linked with photosensors and a laser device using optical fiber. Connecting the photosensors and laser device using optical fibers makes the device more diminutive in size and portable. The prepared sample containing microspheres was passed through the channel, and the surrounding photosensors measured the scattered light. The time-domain features were evaluated from the acquired scattered light, and then the SVM classifier was trained to distinguish the particle's data. The real-time detection of the particles was performed with an overall classification accuracy of 96.06%. The optimum conditions were evaluated to detect the particles with a minimum concentration of 0.2 µg/mL. The developed system is anticipated to be helpful in developing rapid testing devices for detecting pathogens ranging between 2 µm to 10 µm.
Pillararenes are a new type of supramolecular hosts, and they have been widely applied in drug delivery, catalysis, separation process, and sensors. However, they have rarely been used to produce hydrogen. Here, we report that pillararenes were used as functional molecules to explore photocatalysts and efficiently promoted hydrogen production from water. The most common and easily synthesized p-dimethoxy pillar[5]arene (PI-OMe) was employed to form an organic-inorganic hybrid material with titanium dioxide (TiO2), denoted as PI-OMe-TiO2, using a convenient sol-gel method. When the material was loaded with Pt nanoparticles, the resulting Pt/PI-OMe-TiO2 had a good activity and stability in catalyzing water splitting to produce hydrogen under visible light. The optimized catalyst Pt/PI-OMe-TiO2(5.2 wt%) had a photocatalytic hydrogen production rate of 1736 µmol g−1 h−1 under visible light (λ > 420 nm) irradiation. The catalyst with a Pt loading of 0.5 wt% and a PI-OMe content of 5.2 wt% also showed good long-term durability after 10 cycles of 50 h testing. The total amount of hydrogen produced was 65.01 mmol/g, and the corresponding turnover number (TON) value was 2084. Our findings suggest that pillararene derivatives are promising functional molecules to make efficient and stable hybrid photocatalysts with TiO2 and open a new door to hydrogen production using visible light.
A poor biocompatibility and bioactivity of invasive materials remains major problems for biomaterial-based therapy. In this study, we introduced gelatin scaffolds carrying both bone morphogenetic protein-2 (BMP-2) biomimetic peptide and vascular endothelial growth factor-165 (VEGF) that achieved controlled release, cell attachment, proliferation and differentiation. To promote osteogenesis with VEGF, we designed the BMP-2 biomimetic peptide that comprised BMP-2 core sequence oligopeptide (SSVPT), phosphoserine, and synthetic cell adhesion factor (RGDS). In vitro cell experiments, the scaffold was conducive to the adhesion and proliferation of rat bone marrow mesenchymal stem cells (rBMSCs). The micro-CT 3D reconstruction of the rat cranial bone defect model showed that bone regeneration patterns occurred from one side edge towards the center area implanted with the prepared cryogel, and tissue section staining analysis demonstrated that the scaffold with double-growth factor can synergistically accelerate bone regeneration. These findings suggested that the obtained gelatin cryogel could serve as a cell-responsive platform for biomaterial-based nonbearing bone repair.
Both sulfur and fluorine play important roles in organic synthesis, the life science, and materials science. The direct incorporation of these elements into organic scaffolds with precise control of the oxidation states of sulfur moieties is of great significance. Herein, we report the highly selective electrochemical vicinal fluorosulfenylation and fluorosulfoxidation reactions of alkenes, which were enabled by the unique ability of electrochemistry to dial in the potentials on demand. Preliminary mechanistic investigations revealed that the fluorosulfenylation reaction proceeded through a radical-polar crossover mechanism involving a key episulfonium ion intermediate. Subsequent electrochemical oxidation of fluorosulfides to fluorosulfoxides were readily achieved under a higher applied potential with the adventitious H2O in the reaction mixture.
The Cu(I)-catalyzed [4 + 1] annulation of vinyl indoles and a carbene precursor is a powerful method for constructing cyclopentaindole derivatives. Density functional theory (DFT) calculations were used to elucidate the mechanism and regioselectivity of this reaction. After Cu-assisted indole C3-alkylation, direct 1,5-annulation was favored over the Cu-assisted annulation pathway. Furthermore, the regioselectivity for 1,5-annulation was attributed to the generated five-membered-ring product being more stable than the three-membered-ring product from 1,3-annulation, which was the kinetically favored pathway.
The development of innovative strategies and methods to provide natural product-like macrocycles not accessible by biosynthesis, but endowed with novel bioactivities and simplified structure, is highly desirable. Inspired by the key scaffolds of rapamycin and FR252921, herein, we report a Rh(Ⅲ)-catalyzed C-H alkylation macrocyclization, which enables access to CF3-substituted macrolides. DFT calculations reveal that the chemoselectivity between C-H alkylation and olefination macrocyclization was highly controllable. Moreover, the unique CF3-substituted macrolides showed potent anti-inflammation activities against TNF-α, IL-6 and CCL2 mRNA expression.
Artificial membrane transporters that either use chalcogen bonds to facilitate transmembrane flux of anions or show high selectivity toward perchlorate anions are rare. In this work, we report on one such novel monopeptide-based transporter system, featuring both chalcogen bonds for highly efficient anion transport and high transport selectivity toward ClO4- anions. Structurally, these monopeptide molecules associate with each other via H-bonds to produce H-bonded 1D stack that not only one dimensionally but also directionally aligns the terminal bicyclic thiophene motifs to the same side. Functionally, these well-aligned thiophenes create a sulfur-rich transmembrane pathway, combinatorially fine-tunable to enable anions to efficiently cross the membrane in the increasing activity of Cl- < Br- < NO3- < ClO4- via chalcogen bonds, with EC50 values of 0.75, 0.40, 0.37 and 0.093 μmol/L (0.3 mol% relative to lipid molecules), respectively.
Dimeric sesquiterpenoids possessing densely substituted 7-norbornenone/7-norbornenol motifs pose a considerable challenge for chemical synthesis. From a strategic perspective, one could envision intermolecular Diels−Alder cycloaddition as a straightforward method for assembling alkyl-substituted 7-norbornenones. However, this approach is hindered by lability of the required dienes, namely alkyl-substituted cyclopentadienones. Here we report a one-pot protocol for construction of alkyl-substituted 7-norbornenones from electron-deficient olefins and a cyclopentenone derivative. DDQ was found to be an effective oxidant for generating a cyclopentadienone intermediate in situ from the enone. A series of sterically congested 7-norbornenone-containing polycyclic compounds were prepared by using this protocol.
A catalytic asymmetric total synthesis of (+)-vincamine is presented. Key features of the synthesis include a Pd-catalyzed enantioselective decarboxylative allylation to form the C20 quaternary stereogenic center and a stereoselective iminium reduction to install the critical cis-C20/C21 relative stereochemisty.
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