Latest ArticlesAmphichoterpenoids A–C (1–3), unprecedented picoline-derived meroterpenoids possessing a pyrano[3, 2-c]pyridinyl-γ-pyranone scaffold, were characterized from the ascidian-derived fungus Amphichorda felina SYSU-MS7908. Their structures were elucidated by spectroscopic methods, X-ray diffraction and electronic circular dichroism (ECD) calculations. A plausible biosynthetic pathway was proposed. The isolated compounds displayed moderate inhibitory activity against acetylcholinesterase with 50% inhibiting concentration (IC50) values of 18.8–53.2 μmol/L.
The electrocatalysis of nitrate reduction reaction (NRR) has been considered to be a promising nitrate removal technology. Developing a highly effective iron-based electrocatalyst is an essential challenge for NRR. Herein, boron-iron nanochains (B-Fe NCs) as efficient NRR catalysts were prepared via a facile low-cost and scalable method. The Fe/B ratio of the B-Fe NCs-x can be elaborately adjusted to optimize the NRR catalytic performance. Due to the electron transfer from boron to metal, the metal-metal bonds are weakened and the electron density near the metal atom centers are rearranged, which are favor of the conversion from NO3- into N2. Moreover, the well-crosslinked chain-like architectures benefit the mass/electron transport to boost the exposure of abundant catalytic active sites. Laboratory experiments demonstrated that the optimized B-Fe NCs catalyst exhibits superior intrinsic electrocatalytic NRR activity of high nitrate conversion (~80%), ultrahigh nitrogen selectivity (~99%) and excellent long-term reactivity in the mixed electrolyte system (0.02 mol/L NaCl and 0.02 mol/L Na2SO4 mixed electrolyte), and the electrocatalytic activity of the material shows poor performance at low chloride ion concentration (Nitrate conversion of ~61% and nitrogen selectivity of ~57% in 0.005 mol/L NaCl and 0.035 mol/L Na2SO4 mixed electrolyte). This study provides a broad application prospect for further exploring the high-efficiency and low-cost iron-based functional nanostructures for electrocatalytic nitrate reduction.
Vaccine adjuvants have been widely used to enhance the immunogenicity of the antigens and elicit long-lasting immune response. However, only few vaccine adjuvants have been approved by the FDA for human use so far. Therefore, there is still an urgent need to develop novel adjuvants for the potential applications in clinical trials. Herein, non-nucleotide small molecule STING agonist diABZI was employed to construct glycopeptide antigen based vaccines for the first time. Immunological evaluation indicated diABZI not only enhanced the production of antibodies and T cell immune responses, but also inhibited tumor growth in tumor-bearing mice in glycopeptide-based subunit vaccines. These results indicated that di-ABZI demonstrates a high potential as adjuvant for the development of cancer vaccines.
Amino group protective strategy has consequently emerged in multistep organic synthesis. Easy and selective deprotection procedures are crucial to facilitate the chemical transformation. Recently, Zhang's group from Henan Normal University collaborating with Chen's group of Nankai University developed a novel strategy for the regiospecific cleavage of inert aryl C—N bonds in N-aryl amides by hypervalent iodine(V) reagents. These procedures allow removal of sort of aryl groups under mild conditions to give primary amides in high efficiency. It bestows these aryl groups with the characteristics of amino protecting groups that might be the supplement of amino protecting group chemistry.
A nitro group is a common fluorescence quencher, but its quenching efficiency can be easily affected by the surrounding environment. To date, there has been no systematic study on the effects of electron-withdrawing groups on the quenching efficiency of nitro groups. Herein, by virtue of experimental validation and theoretical calculations, we found that strong electron-withdrawing groups, such as pyridinium and dicyanovinyl groups, are detrimental to the quenching effect of nitro groups. Decreasing the electron-withdrawing ability could restore the nitro group's quenching effect.
The remarkable development of nanotechnology and nanoscience has greatly promoted the vigorous development of the field of nanomaterials. This study explores a porous cuboid Ni/NiO composite nanomaterial obtained by calcining NiC2O4·2H2O under a N2 environment. The composite affords direct electrochemical activity and good electrocatalytic properties. Compared to uncalcined precursor, the porous Ni/NiO obtained after calcination exhibited higher catalytic activity for glucose oxidation with higher sensitivity. Moreover, because of its regular cube structure the as-synthesized Ni/NiO exhibited improved electrochemical stability. Such porous Ni/NiO nanocubes represent promising glucose catalyst with high sensitivity and selectivity, improved stability and fast amperometric response.
The construction of nanostructured ion-transport channels is highly desirable in the design of advanced electrolyte materials, as it can enhance ion conductivity by offering short ion-transport pathways. In this work, we present a supramolecular strategy to fabricate a nanocomposite electrolyte containing highly ordered lamellar proton-conducting nanochannels, by the electrostatic self-assembly of a polyoxometalate H3PW12O40 (PW) and a comb copolymer poly(4-methlstyrene)-graft-poly(N-vinyl pyrrolidone). PW can effectively regulate the self-assembling order of polymer moieties to form a large-range lamellar structure, meanwhile, introducing protons into the nanoscale lamellar domains to build proton transport channels. Moreover, the rigid PW clusters contribute a remarkable mechanical reinforcement to the nanocomposites. The lamellar nanocomposite exhibits a conductivity of 4.3×10-4 S/cm and a storage modulus of 1.1×107 Pa at room temperature. This study provides a new strategy to construct nanostructured ion-conductive pathways in electrolyte materials.
The methanol oxidation reaction (MOR) is the limiting half-reaction in direct methanol fuel cell (DMFC). Although Pt is the most active single-metal electrocatalyst for MOR, it is hampered by high cost and CO poisoning. Constructing a Pt or Ru monolayer on a second metal substrate by means of galvanic replacement of underpotentially deposited (UPD) Cu monolayer has been shown as an efficient catalyst design strategy for the electrocatalysis of MOR because of the presumed 100% utilization of atoms and resistance to CO poisoning. Herein, we prepared one-dimensional surface-alloyed electrocatalyst from predominantly (111) faceted Au nanowires with high aspect ratio as the substrate of under-potential deposition. The electrocatalyst comprises a core of the Au nanowire and a shell of catalytically active Pt coated by Ru. Coverage-dependent electro-catalytic activity and stability is demonstrated on the Pt/Ru submonolayers on Au wires for MOR. Among all these catalysts, Au@PtML@RuML exhibits the best electrocatalytic activity and poisoning tolerance to CO. This presents a viable method for the rational catalyst design for achieving high noble-metal utilization efficiency and high catalytic performance.
Encapsulation and controlled release of volatile molecules such as fragrances in a designed manner is important but challenging for the flavor and fragrance industry. Here, we report the tuning release of volatile molecules by postsynthetic modification of an amine-terminated metal-organic framework (MOF) MIL-101-NH2. By amidation, we obtained three MIL-101 MOFs, the trimethylacetamide-terminated TC-MIL-101, the benzamide-terminated BC-MIL-101, and the oxalic acid monoamide-terminated OC-MIL-101. All the MOFs can efficiently encapsulate volatile molecules. Moreover, we demonstrate that the release profile of volatiles can be widely tuned to sustain the release in several days to months and even over a year using different modified MIL-101 MOFs. We show that the release profiles are correlated with the binding energies between the guest volatiles and pores in MOFs. The pore diffusion and the synergistic transport are the rate-limiting step of the guest molecules from the modified MOFs.
Novel and efficient Mn(OAc)3·2H2O promoted radical addition-[4+1] cyclization relay of 3-indolymethanols and phosphites was disclosed, which afforded 1, 2-oxaphospholoindole derivatives in moderate to good yields. Based on the experimental and computational studies, a mechanism involving radical addition and intramolecular cyclization cascade was proposed.
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