Latest ArticlesCovalent organic frameworks (COFs), as a novel class of functional polymers, exhibit versatile applications due to their crystalline porous structures and conjugated skeletons. However, synthesis of COFs with high crystallinity still faces great challenges, especially for scale-up preparation. Herein we report a two-step solvothermal process to improve crystallinity of COFs. The first step focuses on polycondensation of monomers with no need for optimizing crystallization conditions. In the second step, appropriate solvothermal conditions are used to facilitate crystallization of the COFs through defects correction and structural repairing. Furthermore, this strategy could also be applicable to scale-up synthesis of high quality COFs, which lays a foundation for their practical applications.
A novel class of chiral spiro-fused bisoxazoline ligands possessing a deep chiral pocket was prepared. The developed ligands have been employed in the nickel-catalyzed highly enantioselective Michael-type Friedel-Crafts reaction, affording the products bearing a trifluoromethylated all-carbon quaternary stereocenter with moderate to excellent yields (up to 99%) and good to excellent enantioselectivies (up to > 99.9% ee). Moreover, a proposed model of chiral pocket revealed that the attack of indole from the Re-face of β-CF3-β-disubstituted nitroalkene was favorable.
DNA-encoded chemical library (DEL) represents an emerging drug discovery technology to construct compound libraries with abundant chemical combinations. While drug-like small molecule DELs facilitate the discovery of binders against targets with defined pockets, macrocyclic DELs harboring extended scaffolds enable targeting of the protein–protein interaction (PPI) interface. We previously demonstrated the design of the first-generation DNA-encoded multiple display based on a constant macrocyclic scaffold, which harvested binders against difficult targets such as tumor necrosis factor-α (TNF-α). Here, we developed a novel strategy which utilized four orthogonal amine-protecting groups on DNA, to explore larger chemical combinations on the same constant macrocyclic scaffold, following the parallel paradigm to mimic the versatile antibody-like multivalent epitope recognition patterns. We successfully integrated these orthogonal protecting groups with acylation and made a mock second-generation DNA-encoded display combination. This work illustrates a strategy to produce larger encoded multiple display on a constant macrocyclic scaffold, which could facilitate potential binder discovery with enhanced affinity to clinically significant PPI targets.
This brief review reports the recent advancement of metallic glasses and metallic glass nanostructures for functional electrocatalytic applications. Metallic glasses (MGs) or amorphous metals result from quenching the melts at a high cooling rate (e.g., 106 K/s), bypassing crystallization. Metallic glasses are devoid of long-range translational order, no defects like grain boundaries, and multiple elements included. Due to these unique structural features, MG's show distinct and valuable mechanical, physical and chemical properties and therefore were widely studied as a structural material for decades. Even though MGs were proposed for catalytic applications earlier, a comprehensive study or attempt to apply these materials successfully in electrocatalytic applications are few since the intrinsic surface area is comparably lesser. A rejuvenated interest among the research community for applying various novel strategies in catalytic applications of MGs is highlighted in the present review. Theoretical approaches using density functional theory (DFT) and high-throughput screening assisted with machine learning paradigm advances the discovery of new MGs, which demonstrated high potential for catalytic applications. We focus on the basic features and recent advances in the MGs for catalytic applications like electrocatalytic water splitting reactions like HER, OER, fuel cell reactions like ORR, alcohol oxidation reactions like MOR, EOR, and degradation of harmful organic dyes from the industrial effluents. The presently advancing strategies for enhancing the performance of these metallic glass electrocatalysts through nanostructuring and high-throughput screening are discussed. The unique atomic-scale structural mechanism of the metallic glasses, which can favor the development of high-performance electrocatalysts even comparable to currently available precious-metal-based catalysts, will be discussed. Finally, we also give future directions on designing novel and superior metallic glass-based advanced catalysts.
Among the large energy storage batteries, the sodium ion batteries (SIBs) are attracted huge interest due to the fact of its abundant raw materials and low cost, and has become the most promising secondary battery. Tunnel-type sodium manganese oxides (TMOs) are industrialized cathode materials because of their simple synthesis method and proficient electrochemical performance. Na0.44MnO2 (NMO) is considered the best candidate material for all tunnel-type structural materials. In this paper, the research progress in charge and discharge of cathode materials for tunnel-type structural SIBs is reviewed, the redox mechanism and all sorts of synthesis methods and different coating methods lead to different morphology and electrochemical properties of materials and the classification of electrolytes and non-aqueous electrolytes. The development and utility of aqueous solutions are discussed, and the mechanism is analyzed. Summarized the cationic potential of the transition metal oxide for tunnel structure, plays a vital role in predicting and designing the cathode material of this structure. In addition, the future opportunities and challenges for such tunnel-type SIBs in this field are described in detail.
Graphene oxide (GO), as a metal-free and readily available carbocatalyst, has been extensively applied in catalytic organic transformations. This minireview aims to give an overview of the progress on the application of native GO as a catalyst for various organic transformations in the past decade (mainly from 2011 to 2020).
Based on three rationally designed pyrrole-appended o-carborane derivatives, we present that fluorescence properties of crystalline materials are highly dependent on intermolecular interaction and steric hinderance. Though the three molecules are similar in structure, single crystals of the three compounds showed obvious difference in molecular stacking and fluorescence behavior. Systematic studies indicate that fluorescence quantum yields, thermo-response as well as mechano-response are highly dependent on intermolecular interaction and steric hindrance. In the three crystalline materials, the CB-NMe crystals with weaker intermolecular interaction and looser molecular packing showed superior fluorescence quantum yield and temperature sensitivity. Accordingly, surface temperature detection strip with favorable reversibility is prepared by doping CB-NMe into the polymer. In addition, the CB-NMe aggregates can be used for monitoring bovine serum albumin (BSA) denaturation, as temperature response of the aggregates can be reversed when co-assembled with BSA.
In this study, SB216763 and cyclosporine A were identified as anti-influenza A virus (IAV) agents by transcriptome signature reversion (TSR) analysis through deep mining of the cellular transcriptome of human airway and lung cell lines infected with 3 strains of IAV and the chemical perturbations library. A synergistic effect of SB216763 and cyclosporine A against influenza A was disclosed by quantification of the network-based relationship, which was validated in vitro. Along with burgeoning omics approaches, transcriptome-based drug development is flourishing, which provides a novel insight into antivirals discovery with comprehensive cellular transcriptional information of disease and chemical perturbations in multicomponent intervention. This strategy can be applied as a new approach in discovering multitarget antiviral agents from approved drugs, clinical compounds, natural products or other known bioactive compounds.
The asymmetric carbenoid CH insertion of 3-diazooxindoles into 1, 4-cyclohexadiene has been accomplished in the presence of chiral bis(imidazoline) NCN pincer iridium(Ⅲ) complexes as the catalysts. With a catalyst loading of 0.5 mol%, the reactions proceeded smoothly at 0 ℃ to afford a variety of chiral 3-substituted oxindoles in good yields with moderate to excellent enantioselectivities (up to 99% ee). The protocol exhibits good functional group tolerance with respect to 3-diazooxindoles and is readily scaled up to 2 mmol scale without any loss in activity and enantioselectivity. Density functional theory (DFT) calculations have been performed to better understand the reaction mechanism and to explain the stereochemical outcome of the reactions.
Reverse water gas shift (RWGS) reaction is a crucial process in CO2 utilization. Herein, Ni- and NiCe-containing hexagonal mesoporous silica (Ni-HMS and NiCe-HMS) catalysts were synthesized using an in-situ one-pot method and applied for RWGS reaction. At certain reaction temperatures 500-750 ℃, Ni-HMS samples displayed a higher selectivity to the preferable CO than that of conventionally impregnated Ni/HMS catalyst. This could be originated from the smaller NiO nanoparticles over Ni-HMS catalyst. NiCe-HMS exhibited higher activity compared to Ni-HMS. The catalysts were characterized by means of TEM, XPS, XRD, H2-TPR, CO2-TPD, EPR and N2 adsorption-desortion technology. It was found that introduction of Ce created high concentration of oxygen vacancies, served as the active site for activating CO2. Also, this work analyzed the effect of the H2/CO2 molar ratio on the best NiCe-HMS. When reaction gas H2/CO2 molar ratio was 4 significantly decreased the selectivity to CO at low temperature, but triggered a higher CO2 conversion which is close to the equilibrium.
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