Latest ArticlesFive novel biscembranoids, ximaolides H–L (1–5), along with four known related compounds (6–9) were isolated from the Hainan soft coral Sarcophyton tortuosum. The structures of the new compounds were determined by extensive spectroscopic analysis, quantum chemical calculations, and/or by comparing their CD spectra with those of the known compounds. Compounds 1 and 2 are the first examples of biscembranoids bearing a 1,35-bridged lactone moiety, 4 is the first biscembranoid comprising an uncommon oxetane ring, and 5 represents the first 36-peroxyl biscembranoid. Ximaolides I (2), K (4) and F (9) exhibited interesting anti-inflammatory activity by the inhibition of LPS-induced TNF-α protein release in RAW264.7 macrophages.
Carbon nitride (CN) photocatalysts have attracted much attention due to their excellent photocatalytic properties. And hydrothermal fluorination is a common method to improve the photocatalytic effect of CN photocatalyst. Here, the influence of the band gap was first revealed of fluorination and hydroxylation of CN photocatalyst based on the first theoretical principle. Here, the effect of fluorination and hydroxylation on the CN band gap was discussed for the first time using the first theoretical principle. With F atoms and OH doping, the band gap of CN was significantly improved, conduction band and valence band moved up. Then, F—CN photocatalyst with F atoms and OH was successfully synthesized by a hydrothermal fluorinated method. Next, the reasons why F—CN photocatalyst was more effective than that of traditional CN photocatalyst were fully discussed. From the photocatalytic effect of photocatalyst (12, 593.2 μmol g-1 h-1 to the morphology (super-small nanosheets), structure (homojunctions), composition (metal-free), specific surface area (54.1 m2/g), visible light absorption response (AQE is 10.9% at 420 nm) and photo-induced carrier life (14.13 ns). Therefore, this work has a great guiding effect on the development of CN photocatalyst.
SnO2 is considered a promising anode material for sodium-ion batteries due to its high theoretical capacity and low cost. However, the poor electrical conductivity and dramatic volume variation during charge/discharge cycling is a major limitation in its practical applicability. Here we propose a simple one-pot spray pyrolysis process to construct unique pomegranate-like SnO2/rGO/Se spheres. The ideal structural configuration of these architectures was effective in alleviating the large volume variation of SnO2, besides facilitating rapid electron transfer, allowing the devised anode to exhibit superior sodium storage performances in terms of capacity (506.7 mAh/g at 30 mA/g), cycle performance (397 mAh/g after 100 cycles at 50 mA/g) and rate capability (188.9 mAh/g at an ultrahigh current density of 10 A/g). The experimental evidence confirms the practical workability of p-SnO2/rGO/Se spheres in SIBs.
The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry. However, the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism. Here, we report the use of heterogeneous non-noble metal iron nanoparticles (NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory (DFT) method. Fe NPs catalyst displays excellent performance in the dehydrogenation of 1, 2, 3, 4-tetrahydroquinoline (THQ) with 100% selectivity and 100% conversion for 10-12 h at room temperature. The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs. What is more, the energy barrier of transition state is relatively low, illustrating the dehydrogenation is feasible. This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.
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.
Sulfonium salts and sulfur ylides are important S(Ⅳ) motifs, and have displayed many unique reactivities to provide simple, effective, and often stereoselective synthesis toward sulfur containing compounds. Impressive developments have been witnessed within this field during the past several years. In light of the increasing demand of organosulfur compounds across the range of chemical sciences, our aim of this review is to provide a concise overview of recent advances of sulfonium salt and sulfur ylide chemistry. Selected examples are organized in three parts on the basis of their role in organic reactions (reactants, intermediates and catalysts).
As a novel family of macrocyclic molecules, cucurbit[n]urils (CB[n]s) have emerged as promising building blocks of supramolecular nano drug delivery systems (SNDDS) in recent years. Direct encapsulation of amphiphilic guests by CB[6] and CB[7] can modulate their amphiphilicity, resulting in formation of supramolecular amphiphiles that self-assemble into supramolecular nanoparticles for drug delivery. Additionally, CB[n]'s host-guest chemistry on the surface of mesoporous nanoparticles makes CB[n] an ideal blocking agent to control drug release from delivery vehicles. These SNDDS possess intrinsic stimuli responsiveness towards external guest or host, which can further incorporate responsiveness to a variety of other stimuli including pH, thermal, redox, photo and enzyme, to realize multiple stimuli-responsive drug release. Moreover, the recent breakthrough in direct functionalization of CB[n]s has provided a feasible method for preparing superior CB[6] and CB[7] derivatives that can be employed to build multifunctional SNDDS with unoccupied macrocycles located on surface, which could be decorated with various functional "tags" through host-guest chemistry. In this review, we summarized the recent progress of CB[6] and CB[7] based SNDDS through formation of supramolecular amphiphiles, supramolecular nanovalves as well as supramolecularly tailorable surface, which we hope to further promote the development of CB[n]s family as building blocks for advanced SNDDS.
Nickel- and palladium-catalyzed cross-coupling reactions have attracted wide attentions, while ligandcontrolled selectivity in these reactions are still elusive, and calculations can help obtain possible catalytic cycles to generate different products and provide insights into key factors of selectivity, which facilitates the development of new catalyst systems to control reaction selectivity. This review covers our efforts and some significant achievements from other groups on ligand-controlled reaction selectivity of coupling reactions, including introduction, computational methods, selectivity control by ligands in Ni- and Pd-catalyzed coupling reactions, as well as summary and future perspectives.
Incorporation of heteroatoms into the framework of zeolites has become a significant strategy to improve their performance in catalysis and adsorption, because the obtained heteroatom zeolites exhibit quite different properties from the conventional aluminosilicate zeolites in aspects of surface acidity, pore structures, particle size and so on. In this review, the progress on the heteroatom zeolites including their synthesis and application is highlighted. First, the recent advance on the design and synthesis of different heteroatom zeolites is summarized. Special emphasis is placed on the introduction and comparison of three typical methods, including the direct synthesis, post synthesis and improved direct synthesis, for the traditional heteroatom zeolites (such as TS-1, Sn-MFI, Sn-β) and newly-reported heteroatom zeolites (such as W-MFI, Mo-MFI). According to their intrinsic characteristics, the application of heteroatom zeolites in diverse fields, such as production of fine chemicals, air pollution control and biomass conversion is then discussed. Finally, the challenges and perspective on the future development of heteroatom zeolites in low-cost preparation and practical application are proposed.
MXenes, a new family of functional two-dimensional (2D) materials, have shown great potential for an extensive variety of applications within the last decade. Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties. In this review, we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes, and how to control them to directly influence various properties (e.g., electron transport, Li+ adsorption, hydrogen evolution reaction (HER) activity, and magnetism) of 2D MXenes materials. Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed. The review thus provides perspectives on property optimization through atomic defect engineering, and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes.
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