Precisely Controlled Multidimensional Covalent Frameworks: Polymerization of Supramolecular Colloids

Rapid and selective removal of micropollutants from water is important for the reuse of water resources. Despite hollow frameworks with specific functionalized porous walls for the selective adsorption based on a series of interactions, tailoring a stable shape of nanometer- and micrometer-sized architectures for the removal of specific pollutants remains a challenge. Here, exactly controlled sheets, tubes, and spherical frameworks were presented from the crosslinking of supramolecular colloids in polar solvents. The frameworks strongly depended on the architecture of original supramolecular colloids. As the entropy of colloids increased, the initial laminar framework rolled up into hollow tubules, and then further curled into hollow spheres. These shape-persistent frameworks showed unprecedented selectivity as well as specific recognition for the shape of pollutants, thus contributing to efficient pollutant separation.     

Preparation of a novel bentonite intercalation composite by changing the chemical state of aluminum

A new environment-friendly bentonite intercalation composite was successfully obtained from alumina sol intercalation. This process used industrial grade pseudo boehmite as the aluminum source and provided with the advantage of zero emission of acidic wastewater. The bentonite intercalation composite was investigated by XRF, ICP, XRD, FT-IR, BET, and pyridine-FTIR. Results indicated that the basal spacing was enlarged from 14.72 to 15.60 Å; the specific surface area increased by 128%; and the total acid content increased from 65.32 to 245.76 μmol/g. The catalytic activity of this composite was tested by alkylation of aromatics with olefins. The results show that the weak Lewis acid generated by extra-framework aluminum and specific surface area play a decisive role, while weak Brønsted acid site is not the active site for this alkylation reaction.     

Ion pair assisted micro matrix solid phase dispersion extraction of alkaloids from medical plant

A novel micro matrix solid phase dispersion method was successfully used for the extraction of quaternary alkaloids in Phellodendri chinensis cortex. The elution of target compounds was accomplished with sodium hexanesulfonate as the eluent solvent. A neutral ion pair was formed between ion-pairing reagent and positively charged alkaloids in this process, which was beneficial for selectively extraction of polar alkaloids. Several parameters were optimized and the optimal conditions were listed as follows: silica gel as the sorbent, silica to sample mass ratio of 1:1, the grinding time of 1 min. The exhaustive elution of targets was achieved by 200 µL methanol/water (9:1) containing 150 mM sodium hexane sulfonate at pH 4.5. The method validation covered linearity, recovery, precision of intraday and interday, limits of detection, limits of quantitation, and repeatability. This established method was rapid, simple, environmentally friendly, and highly sensitive.     

A detailed investigation into the one-pot cascade reaction of ethyl 3,9-dimethyl-7-phenyl-6H-dibenzo-[b,d]pyran-6-one-8-carboxylate with phenylhydrazine

Research on Chemical Intermediates - When synthesizing cyclohexane-annulated pyrazolones from a cyclohexonedicarboxylate derivative with phenylhydrazine under the catalysis of sulfuric acid in the...     

Aggregation-Induced Synergism by Hydrophobic-Driven Self-Assembly of Amphiphilic Oligonucleotides

The evident contradiction between high local-concentration-based substrate reactivity and free-diffusion-based high reaction efficiency remains one of the important challenges in chemistry. Herein, we propose an efficient aggregation-induced synergism through the hydrophobic-driven self-assembly of amphiphilic oligonucleotides to generate high local concentration whereas retaining high reaction efficiency through hydrophobic-based aggregation, which is important for constructing efficient DNA nanomachines for ultrasensitive applications. MicroRNA-155, used as a model, triggered strand displacement amplification of the DNA monomers on the periphery of the 3D DNA nanomachine and generated an amplified fluorescent response for its sensitive assay. The local concentration of substrates was increased by a factor of at least 9.0×10⁵ through hydrophobic-interaction-based self-assembly in comparison with the traditional homogeneous reaction system, achieving high local-concentration-based reactivity and free-diffusion-based enhanced reaction efficiency. As expected, the aggregation-induced synergism by hydrophobic-driven self-assembly of amphiphilic oligonucleotides created excellent properties to generate a 3D DNA nanomachine with potential as an assay for microRNA-155 in cells. Most importantly, this approach can be easily expanded for the bioassay of various biomarkers, such as nucleotides, proteins, and cells, offering a new avenue for simple and efficient applications in bioanalysis and clinical diagnosis.     

Sustained and Controlled Release of Volatile Precursors for Chemical Vapor Deposition of Graphene at Atmospheric Pressure

Precursors and catalysts play vital roles in chemical reactions. Considerable efforts have been devoted to the investigation of catalysts for graphene growth by chemical vapor deposition in recent years. However, there has been little research on precursors because of a lack of innovation in term of creating a controllable feeding method. Herein, we present a novel sustained and controlled release approach, and develop a convenient, safe, and potentially scalable feeding system with the assistance of matrix materials and a simple portable feeder. As a result, a highly volatile liquid precursor can be fed accurately to grow large-area, uniform graphene films with optimal properties. This feeding approach will further benefit the synthesis of other two-dimensional materials from various precursors.     

Toward Understanding the Enhanced Pseudocapacitive Storage in 3D SnS/MXene Architectures Enabled by Engineered Surface Reactions

The optimization of three-dimensional (3D) MXene-based electrodes with desired electrochemical performances is highly demanded. Here, a precursor-guided strategy is reported for fabricating the 3D SnS/MXene architecture with tiny SnS nanocrystals (≈5 nm in size) covalently decorated on the wrinkled Ti₃C₂T_x nanosheets through Ti−S bonds (denoted as SnS/Ti₃C₂T_x-O). The formation of Ti−S bonds between SnS and Ti₃C₂T_x was confirmed by extended X-ray absorption fine structure (EXAFS). Rather than bulky SnS plates decorated on Ti₃C₂T_x (SnS/Ti₃C₂T_x-H) by one-step hydrothermal sulfidation followed by post annealing, this SnS/Ti₃C₂T_x-O presents size-dependent structural and dynamic properties. The as-formed 3D hierarchical structure can provide short ion-diffusion pathways and electron transport distances because of the more accessible surface sites. In addition, benefiting from the tiny SnS nanocrystals that can effectively improve Na⁺ diffusion and suppress structural variation upon charge/discharge processes, the as-obtained SnS/Ti₃C₂T_x-O can generate pseudocapacitance-dominated storage behavior enabled by engineered surface reactions. As predicted, this electrode exhibits an enhanced Na storage capacity of 565 mAh g⁻¹ at 0.1 A g⁻¹ after 75 cycles, outperforming SnS/Ti₃C₂T_x-H (336 mAh g⁻¹), SnS (212 mAh g⁻¹), and Ti₃C₂T_x (104 mAh g⁻¹) electrodes.     

Metal-Free,Visible-Light-Induced Selective C−C Bond Cleavage of Cycloalkanones with Molecular Oxygen

A metal-free, visible-light-induced oxidative C−C bond cleavage of cycloketones with molecular oxygen is described. Cooperative Brønsted-acid catalysis and photocatalysis enabled selective C−C bond cleavage of cycloketones to generate an array of γ-, δ- and ϵ-keto esters under very mild conditions. Mechanistic studies indicate that singlet molecular oxygen (¹O₂) is responsible for this transformation.