Latest ArticlesThe cheap and easily available sodium dithionite and thiourea dioxide have been used as the source of sulfonyl group in the synthesis of sulfones and sulfonamides recently. Compared with other methods for the sulfonylation reactions, the strategies using sodium dithionite or thiourea dioxide provide an alternative and complementary route to diverse sulfonyl compounds. During the reaction process, sulfur dioxide anion radical is the key intermediate, which is usually generated from a single electron transfer under suitable conditions. The advantages using sodium dithionite or thiourea dioxide in the sulfonylation reactions include mild conditions and broad substrate scope with excellent functional group compatibility. Further applications by using sodium dithionite and thiourea dioxide in organic transformations will be anticipated.
Oxygen evolution reaction (OER) is admitted to an important half reaction in water splitting for sustainable hydrogen production. The sluggish four-electron process is known to be the bottleneck for enhancing the efficiency of OER. In this regard, tremendous efforts have been devoted to developing effective catalysts for OER. In addition to Ir- or Ru-based oxides taken as the benchmark, transition metal carbides have attracted ever-increasing interest due to the high activity and stability as low-cost OER electrocatalysts. In this review, the transition metal carbides for water oxidation electrocatalysis concerning design strategies and synthesis are briefly summarized. Some typical applications for various carbides are also highlighted. Besides, the development trends and outlook are also discussed.
For bone regenerative engineering, it is a promising method to form skeletal tissues differentiating from human bone morrow mesenchyme stem cells (hBMSCs). However, it is still a critical challenge to efficiently control ostogenesis and clearly reveal the influence factor. To this end, the fluorescent gold nanodots (Au NDs) with highly negative charges as osteogenic induction reagent are successfully synthesized, which display better than commercial osteogenic induction medium through the investigations of ALP activity (2.5 folds) and cytoskeleton staining (1.5 folds). Two kinds of oligopeptides with different bio-structures (cysteine, Cys and glutathione, GSH) are selected for providing surficial charges on Au NDs. It is revealed that Au-Cys with more negative charges (-51 mV) play better role than Au-GSH (-19 mV) in osteogenic differentiation, when both of them have same size (~2 nm), sphere shape and show similar cell uptake amount. To explore deeply, osteogenesis related signaling pathways are monitored, revealing that the enhancement of osteogenic differentiation was through autophagy signaling pathway triggered by Au-Cys. And the promotion of highly negative charges in osteogenic differentiation was further proved via sliver nanodots (Ag NDs, Ag-Cys and Ag-GSH) and carbon nanodots (CDs, Cys-CDs and GSH-CDs). This work indicates part of insights during hBMSCs differentiation and provides a novel strategy in osteogenic differentiation process.
Porous carbon spheres represent an ideal family of electrode materials for supercapacitors because of the high surface area, ideal conductivity, negligible aggregation, and ability to achieve space efficient packing. However, the development of new synthetic methods towards porous carbon spheres still remains a great challenge. Herein, N-doped hollow carbon spheres with an ultrahigh surface area of 2044 m2/g have been designed based on the phenylenediamine-formaldehyde chemistry. When applied in symmetric supercapacitors with ionic electrolyte (EMIBF4), the obtained N-doped hollow carbon spheres demonstrate a high capacitance of 234 F/g, affording an ultrahigh energy density of 114.8 Wh/kg. Excellent cycling stability has also been achieved. The impressive capacitive performances make the phenylenediamine-formaldehyde resin derived N-doped carbon a promising candidate electrode material for supercapacitors.
Metal-free direct α-C(sp3)—H intramolecular cyclization of 2-alkylthiobenzoic acid in the presence of Selectfluor is described. This novel strategy provides a facile and efficient method to access important 1, 3-benzooxathiin-4-one derivatives with good functional groups tolerance and yields.
In this research, a hydroxyl group functionalized metal-organic framework (MOF), UiO-66-(OH)2, was synthesized as a "on-off-on" fluorescent switching nanoprobe for highly sensitive and selective detection of Fe3+, ascorbic acid (AA) and acid phosphatase (ACP). UiO-66-(OH)2 emits yellow-green light under ultraviolet light, when Fe3+ was added, Fe3+ was chelated with hydroxyl group, the electrons in the excited state S1 of the MOF transferred to the half-filled 3d orbits of Fe3+, resulting in fluorescence quenching because of the nonradiative electron/hole recombination annihilation. AA could reduce Fe3+ to Fe2+, which can destroy the electron transfer between UiO-66-(OH)2 and Fe3+ after AA adding, resulted in nonoccurrence of the nonradiative electron transfer, leading to the recovery of UiO-66-(OH)2 fluorescence intensity. The probe can also be used to detect ACP based on the enzymolysis of 2-phospho-L-ascorbic acid (AAP) to produce AA. Benefitting from the hydroxyl group and the characteristics of UiO-66, including the high porosity and large surface area, the developed UiO-66-(OH)2 showed extensive advantages as a fluorescent probe for detection of multi-component, such as high sensitivity and selectivity, colorimetric detection, fast response kinetics and easy to operate, economical and secure. This is the first time to use active group functionalized MOFs as a multi-component sensor for these three substances detection.
Integrating silica with organic nanoparticles can generate unique properties. Here pillar[5]arene/silica hybrid vesicles were constructed based on the amphiphilic and rigid properties of pillararenes, as well as the catalytic hydrolysis of tetraethoxysilane. Such vesicles exhibited the high strength of silica and unique molecular recognition of pillararenes, both of which could tune the pH-triggered release behavior. Furthermore, a rhodamine B derivative with hexyl group (RhB-C6) was synthesized, which can form a complex with the pillar[5]arene. Based on the host-guest interaction and high strength of silica, the hybrid vesicles could load more RhB-C6 and the rhodamine B was released more slowly compared with the organic vesicles.
Single atom catalysts (SACs) with isolated metal atoms dispersed on supports exhibit distinctive performances for electrocatalysis reactions. The designable realization of well-dispersed single metal atoms is still a great challenge owing to their ease of aggregation. Here, Mo single atomic sites (Mo-N3C) combined with some ultrasmall Mo2C/MoN clusters (Mo-SA/Mo2C-MoN-Cs, mean diameter < 2 nm) on nitrogen-doped porous carbon were synthesized via a simple pyrolysis of bimetallic Zn/Mo metal-organic frameworks. X-ray absorption near edge spectra (XANES) in combination with various characterizations show that most of Mo species in sample exist in the form of single sites and the exact structure is Mo-N3C. Density functional theory (DFT) calculation further shows that as the number of N-coordination in the Mo-NxC moieties increases, the positive charge of Mo atoms increases. The single Mo atoms in Mo-N3C have the best capability of N2 adsorption, which may serve as main active sites for further electrochemical N2 reduction.
Hollow nanostructures have attracted increasing research interest in hydrogen evolution reaction owing to their unique structural features. Herein, Ni–Co mixed metal phosphide hollow and porous polyhedrons was successfully composited (expressed as NiCoP). Benefiting from the synergistic effects of ZIF-67 by doping Ni elements and the well-defined hollow and porous structure, the as-synthesized NiCoP hollow and porous polyhedrons exhibit better electrochemical properties and mechanical stability for hydrogen evolution reaction over a pH-universal range, with a small Tafel slopes of 72, 101, 176 mV/dec, and a low overpotential of 82, 102, 261 mV at a current density of 10 mA/cm2 in 0.5 mol/L H2SO4, 1 mol/L KOH and 1 mol/L phosphate buffer solution (PBS). This general strategy can also be applied to fabricate other hollow cobalt-based phosphides and MOFs-derived materials for HER.
Based on the crystal structures of two cucurbit[6]uril/calix[n]arene-based supramolecular frameworks reported by Long and co-workers, we further investigated the interactions of cucurbit[6]uril with 4-sulfocalix[4]arene and 4-sulfocalix[6]arene using 1H NMR spectroscopy and isothermal titration calorimetry (ITC), respectively. Moreover, solid fluorescent materials were prepared via the adsorption of fluorescent dyes by these porous supramolecular frameworks, which exhibit a selective response to certain volatile organic compounds.
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