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Nat Commun ; 8: 14460, 2017 02 16.
Artigo em Inglês | MEDLINE | ID: mdl-28205528


It is highly desirable to reduce the membrane thickness in order to maximize the throughput and break the trade-off limitation for membrane-based gas separation. Two-dimensional membranes composed of atomic-thick graphene or graphene oxide nanosheets have gas transport pathways that are at least three orders of magnitude higher than the membrane thickness, leading to reduced gas permeation flux and impaired separation throughput. Here we present nm-thick molecular sieving membranes composed of porous two-dimensional metal-organic nanosheets. These membranes possess pore openings parallel to gas concentration gradient allowing high gas permeation flux and high selectivity, which are proven by both experiment and molecular dynamics simulation. Furthermore, the gas transport pathways of these membranes exhibit a reversed thermo-switchable feature, which is attributed to the molecular flexibility of the building metal-organic nanosheets.

ACS Appl Mater Interfaces ; 8(28): 18505-12, 2016 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-27385672


It is challenging to introduce pendent sulfonic acid groups into modularly built crystalline porous frameworks for intrinsic proton conduction. Herein, we report the mechanoassisted synthesis of two sulfonated covalent organic frameworks (COFs) possessing one-dimensional nanoporous channels decorated with pendent sulfonic acid groups. These COFs exhibit high intrinsic proton conductivity as high as 3.96 × 10(-2) S cm(-1) with long-term stability at ambient temperature and 97% relative humidity (RH). In addition, they were blended with nonconductive polyvinylidene fluoride (PVDF) affording a series of mixed-matrix membranes (MMMs) with proton conductivity up to 1.58 × 10(-2) S cm(-1) and low activation energy of 0.21 eV suggesting the Grotthuss mechanism for proton conduction. Our study has demonstrated the high intrinsic proton conductivity of COFs shedding lights on their wide applications in proton exchange membranes.

Chem Commun (Camb) ; 52(52): 8087-90, 2016 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-27181340


We report the intergrowth of ZIF-8 crystals on ultrathin graphene oxide (GO) membranes, which helps to reduce the non-selective pores of pristine GO membranes leading to gas selectivities as high as 406, 155, and 335 for H2/CO2, H2/N2, and H2/CH4 mixtures, respectively.

ACS Appl Mater Interfaces ; 5(23): 12554-60, 2013 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-24245853


Increasing attention has been given to nanobiocatalysis for commercial applications. In this study, laccase was immobilized on polyacrylonitrile (PAN) nanofibrous membranes through ethanol/HCl method of amidination reaction and successfully applied for removal of 2,4,6-trichlorophenol (TCP) from water. PAN membranes with fiber diameters from 200 nm to 300 nm were fabricated via electrospinning and provided a large surface area for enzyme immobilization and catalytic reactions. Images of scanning electron microscope demonstrated the enzyme molecules were aggregated on the nanofiber surface. The immobilized laccase exhibited 72% of the free enzyme activity and kept 60% of its initial activity after 10 operation cycles. Moreover, the storage stability of the immobilized laccase was considered excellent because they maintained more than 92% of the initial activity after 18 days of storage, whereas the free laccase retained only 20%. The laccase-PAN nanofibrous membranes exhibited high removal efficiency of TCP under the combined actions of biodegradation and adsorption. More than 85% of the TCP was removed under optimum conditions. Effects of various factors on TCP removal efficiency of the immobilized laccase were analyzed. Results suggest that laccase-PAN nanofibrous membranes can be used in removing TCP from aqueous sources and have potential for use in other commercial applications.

Resinas Acrílicas/química , Clorofenóis/química , Lacase/química , Membranas Artificiais , Nanofibras , Concentração de Íons de Hidrogênio , Microscopia Eletrônica de Varredura , Espectroscopia de Infravermelho com Transformada de Fourier , Temperatura
Bioresour Technol ; 149: 111-6, 2013 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-24096278


Horseradish peroxidase (HRP) from roots of horseradish (Amoracia rusticana) was successfully immobilized on novel enzyme carriers, poly(methyl methacrylate-co-ethyl acrylate) (PMMA CEA) microfibrous membranes, and used for removal of bisphenol A from water. PMMA CEA fibrous membranes (PFM) with fiber diameters of 300-500 nm, were fabricated by electrospinning. HRP was covalently immobilized on the surface of microfibers previously activated by polyethylenimine and glutaraldehyde. HRP loading reached 285 mg/g, and enzyme activity was 70% of free HRP after immobilization. Both stabilities and reusability of HRP were greatly improved after immobilization. After six repeated runs, immobilized HRP retained about 50% of its initial activity. Immobilized HRP exhibited significantly higher removal efficiency for bisphenol A (BPA) in 3h (93%) compared with free HRP (61%) and PFM alone (42%). The high BPA removal can be resulted by improvement of catalytic activity of immobilized HPR with adsorption on modified PMMA CEA support.

Resinas Acrílicas/química , Compostos Benzidrílicos/isolamento & purificação , Enzimas Imobilizadas/metabolismo , Peroxidase do Rábano Silvestre/metabolismo , Membranas Artificiais , Fenóis/isolamento & purificação , Polimetil Metacrilato/química , Adsorção , Biodegradação Ambiental , Estabilidade Enzimática , Concentração de Íons de Hidrogênio , Cinética , Temperatura , Fatores de Tempo , Poluentes Químicos da Água/isolamento & purificação