Anhydrous interfacial polymerization of sub-1 Å sieving polyamide membrane.

Highly permeable polyamide (PA) membrane capable of precise ionic sieving can be utilized for many energy-efficient chemical separations. To fulfill this target, it is crucial to innovate membrane-forming process to induce a narrow pore-size distribution. Herein, we report an anhydrous interfacial polymerization (AIP) at a solid-liquid interface where the amine layer sublimated is in direct contact with the alkane containing acyl chlorides. In such a heterophase interface, water-caused side reactions are eliminated, and the amines in compact arrangement enable an intensive and orderly IP reaction, leading to a unique PA layer with an ionic sieving accuracy of 0.5 Å. The AIP-PA membrane demonstrates excellent separation selectivities of monovalent and divalent cations such as Mg2+/Li+ (78.3) and anions such as Cl-/SO42- (29.2) together with a high water flux up to 13.6 L m-2 h-1 bar-1. Our AIP strategy may provide inspirations for engineering high-precision PA membranes available in various advanced separations.

Ultra-Fast Preparation of Large-Area Graphdiyne-Based Membranes via Alkynylated Surface-Modification for Nanofiltration.

Graphdiynes (GDYs), two-dimensional graphene-like carbon systems, are considered as potential advanced membrane material due to their unique physicochemical features. Nevertheless, the scale-up of integrated GDY membranes is technologically challenging, and most studies remain at the theoretical stage. Herein, we report a simple and efficient alkynylated surface-mediated strategy to prepare hydrogen-substituted graphdiyne (HsGDY) membranes on commercial alumina tubes. Surface alkynylation initiates an accelerated surface-confined coupling reaction in the presence of a copper catalyst and facilitates the nanoscale epitaxial lateral growth of HsGDY. A continuous and ultra-thin HsGDY membrane (∼100 nm) can be produced within 15 min. The resulting membranes exhibit outstanding molecular sieving together with excellent water permeances (ca. 1100 L m-2 h-1 MPa-1 ), and show a long-term durability in cross-flow nanofiltration, owing to the superhydrophilic surface and hydrophobic pore walls.

Molecular Dynamics Simulations of the Oil-Detachment from the Hydroxylated Silica Surface: Effects of Surfactants, Electrostatic Interactions, and Water Flows on the Water Molecular Channel Formation.

The detachment process of an oil molecular layer situated above a horizontal substrate was often described by a three-stage process. In this mechanism, the penetration and diffusion of water molecules between the oil phase and the substrate was proposed to be a crucial step to aid in removal of oil layer/drops from substrate. In this work, the detachment process of a two-dimensional alkane molecule layer from a silica surface in aqueous surfactant solutions is studied by means of molecular dynamics (MD) simulations. By tuning the polarity of model silica surfaces, as well as considering the different types of surfactant molecules and the water flow effects, more details about the formation of water molecular channel and the expansion processes are elucidated. It is found that for both ionic and nonionic type surfactant solutions, the perturbation of surfactant molecules on the two-dimensional oil molecule layer facilitates the injection and diffusion of water molecules between the oil layer and silica substrate. However, the water channel formation and expansion speed is strongly affected by the substrate polarity and properties of surfactant molecules. First, only for the silica surface with relative stronger polarity, the formation of water molecular channel is observed. Second, the expansion speed of the water molecular channel upon the ionic surfactant (dodecyl trimethylammonium bromide, DTAB and sodium dodecyl benzenesulfonate, SDBS) flooding is more rapidly than the nonionic surfactant system (octylphenol polyoxyethylene(10) ether, OP-10). Third, the water flow speed may also affect the injection and diffusion of water molecules. These simulation results indicate that the water molecular channel formation process is affected by multiple factors. The synergistic effects of perturbation of surfactant molecules and the electrostatic interactions between silica substrate and water molecules are two key factors aiding in the injection and diffusion of water molecules and helpful for the oil detachment from silica substrate.

Molecular dynamics simulations of the self-organization of side-chain decorated polyaromatic conjugation molecules: phase separated lamellar and columnar structures and dispersion behaviors in toluene solvent.

The self-organization of five model side-chain decorated polyaromatic asphaltene molecules with or without toluene solvent was investigated by means of atomistic molecular dynamic (MD) simulations. It was found that the organizational structure of polycyclic asphaltene molecules is significantly affected by the position and length of side chains. In the present study, two types of phase-separated stacking configurations, including the phase separated lamellar structure (PSLS) and the phase separated columnar structure (PSCS), were found. The PSLS and PSCS were also maintained in the presence of a small amount of toluene additive (30% wt fraction). When adding excess toluene molecules, the asphaltene molecules formed highly dispersed nanoaggregates. The dynamic properties of the π-π stacking structures in the PSLS and PSCS, as well as the nanoaggregates, were probed. It was found that the number and size of alkyl side chains significantly impacted the size and number of π-π stacking structures in the aggregates. Through tracking the structural evolution of the nanoaggregates, a possible dissociation mechanism of nanoaggregates is also suggested.

Construction of a trans-splicing ribozyme for restoring EGFP truncation mutation / 生物工程学报

Special designed group I intron ribozymes can specifically splice objective RNA, repair the mutant gene in RNA level. The specificity of ribozyme is determined by nucleotides specific internal guide sequence (IGS) introduced to the enzyme. In this study, fragment sequence containing Tetrahymena thermophilia intron I of 26S rRNA gene was cloned and cis-splicing activity of this ribozyme was confirmed by in vitro transcription. For evaluating the trans-splicing activity of this ribozyme, a truncated mutant Green Fluorescence Protein (GFP) vector, XYQ5/XYQ10- pEGFP-C2, was constructed. This vector deleted the 3' end 564bp fragment of EGFP coding sequence, led to the lost the activity of emitting green fluorescence. Trans-splicing ribozyme plasmids ptrans-rib-CMV2 for remedy of the truncated mutant EGFP was constructed by PCR and molecular cloning techniques. This vector utilizing cloned 26S rRNA intron 1 as core enzyme; selecting T-G site at 194bp of EGFP coding sequence as splicing receptor, designed an IGS which is inversely complement to the 188-193nt of EGFP mRNA; the 195-890bp fragment of EGFP coding sequence was ligated to the 3'-end of ribozyme core. The fragment containing these components was inserted to a eukayotic expression vector pRC-CMV2. Using linearized XYQ5/XYQ10- pEGFP-C2 and ptrans-rib-CMV2 as templates, truncated EGFP mRNA and the constructed ribozyme vector were transcribed and mixed to evaluate the trans-splicing activity. Analysis of in vitro transcription products mix by RT-PCR verified the existence of wild type EGFP mRNA molecule. Co-transfection of XYQ5/XYQ10- pEGFP-C2 with ptrans-rib-CMV2 to Hela cells proved this ribozyme restored green fluorescence within cell, but the efficiency was low.