Abstract ：

BackgroundAbnormally regulated long non-coding RNAs (lncRNAs) functions in cancer emphasize their potential to serve as potential targets for cancer therapeutic intervention. LncRNA ASBEL has been identified as oncogene and an anti-sense transcript of tumor-suppressor gene of BTG3 in triple-negative breast cancer (TNBC).ResultsHerein, multicomponent self-assembled polyelectrolyte nanocomplexes (CANPs) based on the polyelectrolytes of bioactive hyaluronic acid (HA) and chitosan hydrochloride (CS) were designed and prepared for the collaborative modulation of oncogenic lncRNA ASBEL with antago3, an oligonucleotide antagonist targeting lncRNA ASBEL and hydrophobic curcumin (Cur) co-delivery for synergetic TNBC therapy. Antago3 and Cur co-incorporated CANPs were achieved via a one-step assembling strategy with the cooperation of noncovalent electrostatic interactions, hydrogen-bonding, and hydrophobic interactions. Moreover, the multicomponent assembled CANPs were ulteriorly decorated with a near-infrared fluorescence (NIRF) Cy-5.5 dye (FCANPs) for synchronous NIRF imaging and therapy monitoring performance. Resultantly, MDA-MB-231 cells proliferation, migration, and invasion were efficiently inhibited, and the highest apoptosis ratio was induced by FCANPs with coordination patterns. At the molecular level, effective regulation of lncRNA ASBEL/BTG3 and synchronous regulation of Bcl-2 and c-Met pathways could be observed.ConclusionAs expected, systemic administration of FCANPs resulted in targeted and preferential accumulation of near-infrared fluorescence signal and Cur in the tumor tissue. More attractively, systemic FCANPs-mediated collaborative modulating lncRNA ASBEL/BTG3 and Cur co-delivery significantly suppressed the MDA-MB-231 xenograft tumor growth, inhibited metastasis and extended survival rate with negligible systemic toxicity. Our present study represented an effective approach to developing a promising theranostic platform for combating TNBC in a combined therapy pattern.

Keyword ：

LncRNA ASBEL Triple-negative breast cancer Synchronous theranostics Polyelectrolyte nanocomplexes Curcumin Self-assembled

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Abstract ：

Assembling two-dimensional (2D) materials by polyelectrolyte often suffers from inhomogeneous microstructures due to the conventional mixing-and-simultaneous-complexation procedure ("mix-and-complex") in aqueous solution. Herein a "mix-then-on-demand-complex" concept via on-demand in situ cascade anionization and ionic complexation of 2D materials is raised that drastically improves structural order in 2D assemblies, as exemplified by classical graphene oxide (GO)-based ultrathin membranes. Specifically, in dimethyl sulfoxide, the carboxylic acid-functionalized GO sheets (COOH-GOs) were mixed evenly with a cationic poly(ionic liquid) (PIL) and upon filtration formed a well-ordered layered composite membrane with homogeneous distribution of PIL chains in it; next, whenever needed, it was alkali-treated to convert COOH-GO in situ into its anionized state COO--GO that immediately complexed ionically with the surrounding cationic PIL chains. This "mix-then-on-demand-complex" concept separates the ionic complexation of GO and polyelectrolytes from their mixing step. By synergistically combining the PIL-induced hydrophobic confinement effect and supramolecular interactions, the as-fabricated nanofiltration membranes carry interface transport nanochannels between GO and PIL, reaching a high water permeability of 96.38 L m(-2) h(-1) bar(-1) at a maintained excellent dye rejection 99.79% for 150 h, exceeding the state-of-the-art GO-based hybrid membranes. The molecular dynamics simulations support the experimental data, confirming the interface spacing between GO and PIL as the water transport channels.

Keyword ：

confinement effect nanofiltration poly(ionic liquid) graphene oxide ionic complexation

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Abstract ：

The membrane fouling is a notorious problem in the practical application of separation membranes. In this study, a mixed matrix membrane based on the MOF BUT-8(A) and the polymer polydiallyldimethylammonium chloride (PDDA) has been prepared on a hydrolyzed polyacrylonitrile (HPAN) substrate by the spinassisted layer-by-layer assembly (spin-LbL) method. Thanks to the high porosity, high stability, moderate hydrophilicity, and electronegative nature of BUT-8(A), and the good compatibility between BUT-8(A) particles and PDDA polyelectrolytes, the prepared (BUT-8(A)/PDDA)3-HPAN membrane showed high water permeances (over 164 L m(-2) h(-1) MPa-1) and high rejection rates (over 91.4%) for many dyes in water. Furthermore, the membrane exhibited superior antifouling performance in nanofiltration (NF) with a high flux recovery rate (95.5%) when humic acid (HA) was used as foulant. The high antifouling performance is resulted from tuning hydrophilicity and electronegativity of the membrane surface. These results suggest that the nanofiltration performance of a MOF-based membrane can be well adjusted by a judicious choice of the membrane components and fabrication methods. (c) 2020 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

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Metal-organic framework (MOF) Layer-by-layer assembly Nanofiltration Mixed matrix membrane

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A bio-polyelectrolyte (PC) was synthesized by reacting phytic acid (PA) with casein (CS), and used as the shell materials to microencapsulate ammonium polyphosphate (APP). The obtained core-shell structured flame retardant (PC@APP) was incorporated into polylactic acid (PLA). The dispersion of PC@APP was greatly improved. As a result, the elongation at break and notched impact strength were improved from 6.9% and 3.5 KJ/m(2) of neat PLA sample to 14.4% and 4.7 KJ/m(2) of PLA samples containing 5%PC@APP. Moreover, the fire resistance of PLA/5%PC@APP composites was also enhanced. The limiting oxygen index (LOI) value was increased from 19.6% to 28.3%; the vertical burning (UL-94) rating was upgraded from no rating to V-0; and the peak heat release rate value was decreased from 935.8 kW/m(2) to 747.9 kW/m(2). It is suggested that the well-dispersed PC@APP alters the degradation routine of PLA matrix, leading to the rapid formation of physical barriers.

Keyword ：

Microencapsulation Flame retardancy Bio-polyelectrolytes Polylactic acid composites

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The layered transition metal dichalcogenides, molybdenum disulfide (MoS2) have received increasing attention and hold great potential applications in various fields due to its unique properties. In this work, the PDDA modified MoS2 nanosheets (PDDA@MoS2 nanosheets) were prepared and then incorporated into polyelectrolyte multilayers through layer-by-layer self-assembly method to get a PDDA@MoS2-PDDA/PSS hybrid membrane. The morphologies and structures of the resulted PDDA@MoS2 nanosheets and hybrid membranes were characterized by X-ray diffraction, scanning electron microscope, transmission electron microscopy, X-ray photoelectron spectroscopy, energy dispersive spectroscopy and atom force microscopy. The nanofiltration performance of the hybrid membranes were investigated by retention of dyes and salts from aqueous solution. The result indicated that the hybrid membranes showed 98.4% retention of methyl blue with flux of 194.4 L/m(2) h MPa, which was 2.3 times than that of pure poly electrolytes membrane with flux of 82.7 L/m(2) h MPa. And the hybrid membrane also showed rejection of salts in the sequence Na2SO4 > MgSO4 > NaCl > MgCl2. Moreover, the flux of the membrane remained around 180.0 L/m(2) h MPa, while the rejection was maintained at about 98.0% during the 165 h running time, displaying good long term stability. (C) 2018 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keyword ：

PDDA@MoS2 nanosheets Hybrid membrane Nanofiltration

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A superhydrophilic poly (ethyleneimine)/poly (acrylicacid) PEI/PAA-Cerium carbonate (Ce-2(CO3)(3)) composite membrane was fabricated through layer-by-layer (LbL) self-assembly and in situ mineralization of Ce-2(CO3)(3). The surface structures, wetting behavior and NF performance of the membranes were investigated. The results indicated that the water contact angle of [PEI/PAA-Ce-2(CO3)](3.0) membrane decreased with increasing incorporated Ce-2(CO3)(3) content. Under 0.025 mol/L of Ce-2(CO3)(3) content, the prepared membrane showed superhydrophilic surface with water contact angle of 3.1 degrees, which can effectively separate methyl blue, xylenol orange and eriochrome black T from aqueous solution with rejection of more than 95% and flux of more than 152.0 L/m(2) MPa h, respectively. In addition, the superhydrophilic membrane showed better long-term running stability, and antifouling property. After 3 cycle of running and cleaning, the flux recovery rate was about 85%, and the irreversible flux decay rate was 14.53%. Moreover, the Derjaguin Landau Verwey Overbeek (XDLVO) approach further demonstrated that the superhydrophilic membrane showed higher antifouling property than the hydrophilic one. (C) 2018 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keyword ：

Polyelectrolytes Nanofiltration Superhydrophilic membrane Antifouling effect Cerium carbonate

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Abstract ：

Graphene oxide has great potentials for preparing multilayers with polyelectrolytes due to its abundant carboxyl groups. The as-resulting polyelectrolyte multilayers (PEMs) showed excellent performance and significant improved stability in membrane separation applications. However, the stability enhancement of GO nanosheets in the GO incorporated PEMs is still lack of systematic discussion. In this study, the enhancements of GO were confirmed by comparing the pristine and GO incorporated PEMs membranes through layer-by-layer self-assembly strategy. The membranes were post-treated with NaCIO/NaOH/HCI solutions, and the morphologies, chemical properties, and separation capabilities of the multilayer membranes before and after treatment were compared. The results indicate that the probable mechanism for the enhancements is attributed to the confinement effects of GO nanosheets on the migration and rearrangement of polyelectrolyte chains. Thus, we anticipate that this study could provide a comprehensive understanding of GO based multilayers and an approach to prepare stable PEMs membranes with GO nanosheets and other 2D materials.

Keyword ：

Confinement effect Layer-by-layer self-assembly Polyelectrolyte multilayer "Brick-and-mortar" structure Graphene oxide nanosheet

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Superhydrophilic poly(ethyleneimine)/poly(sodium-4-styrenesulfonate) (PEI/PSS)-calcium silicate hydrate (CSH) multilayered membranes (PEI/PSS)(2.0)(PEI/PSS-CSH)(n) on polyacrylonitrile (PAN) substrate were prepared via layer-by-layer (LbL) assembly with in situ precipitation of consecutive Ca2+-integrated multilayered polyelectrolytes and sodium silicate. The surface structure and properties of these multilayered membranes (PEI/PSS)(2.0)(PEI/PSS-CSH)(n) were characterized by zeta potential, infrared resonance spectra, water contact angles, scanning electron microscopy, and atomic force microscopy, and the separation performances were evaluated by rejection of dyes, such as xylenol orange (XO) and rhodamine B (RB). The long term performance, self-cleaning and antifouling behaviors were investigated by retention of aqueous solutions of both dyes and bovine serum albumin (BSA) aqueous solution. The results indicated that the in situ incorporation of controlled CSH contents into PEI/PSS multilayers greatly improved the hydrophilicity of the multilayered membranes, resulting in the formation of a superhydrophilic (PEI/PSS-CSH)(2.0) membrane with a water contact angle of 2.1 degrees and the highest permeate fluxes of 191.5 and 183.5 L m(-2) h(-1) MPa-1 accompanied by the rejection of 94.0% and 91.2% for XO and RB aqueous solutions, respectively. When the number of assembled (PEI/PSS-CSH)(n) multilayers was higher than 2.0 bilayers, the rejection increased but the flux markedly decreased to XO and RB dyes, showing a characteristic trade-off phenomenon. Moreover, the superhydrophilic (PEI/PSS-CSH)(2.0) membrane possessed a higher antifouling and self-cleaning behavior than the hydrophilic polyelectrolytes (PEI/PSS)(2.0).

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Abstract ：

Nanofiltration membrane was prepared by static layer-by-layer (LBL) self-assembly of poly(ethyleneimine) (PEI) and poly(sodium 4-styrenesulfonate) (PSS) on the modified poly-arcylonitrile ultra-filtration membrane. Study on self-assembly of polyelectrolyte membranes with changing surface charges and wettability, rejection properties of nanofiltration membrane in different conditions and pH with respect to heavy metal ions, namely Ni2+ and Cd2+were investigated. The results show that the PEI/PSS membrane composed of 4 bilayers at operating pressure 0.4MPa, rejection of PAN-PEI/PSS nanofiltration membrane towards these 2 kind of heavy metal ions reached no less than 90%. © (2014) Trans Tech Publications, Switzerland.

Keyword ：

Nanofiltration Metal ions Polyelectrolytes Nanofiltration membranes Heavy metals Self assembly

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Abstract ：

Alternating layer-by-layer (LbL) deposition of polycations and polyanions on porous substrates is a convenient and versatile method for forming high-flux nanofiltration (NF) membranes. In this work, positively charged NF membranes were fabricated by the LbL assembly of poly (ethyleneimine) (PEI) and poly(sodium 4-styrenesulfonate) (PSS) on the modified polyacrylonitrile ultra-filtration substrate. The charge variation with each layer was characterized by zeta potential. ATR-FTIR, SEM, N-2 adsorption and the weight changes with bi-layers were used to confirm the LbL deposition of the polyelectrolytes. NF performances of the prepared membrane with a number of bi-layers as well as solute concentrations were also investigated. The results of zeta potential showed that the whole multilayer films exhibited periodic variations in positive charge. NF results indicated that the rejection of Ni2+ and Cd2+ ions increased, while the permeate fluxes decreased with the number of bi-layers. And the rejections of the metal ion solutes were 98.02% for CuSO4, 95.53% for ZnSO4, 95.66% for NiCl2, 94.9% for CdCl2, along with permeation fluxes of 19.02, 19.72, 24.02, and 21.19 L/m(2).h, respectively.

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