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1.
Small ; : e2402105, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38727184

ABSTRACT

The scarcity of fresh water necessitates sustainable and efficient water desalination strategies. Solar-driven steam generation (SSG), which employs solar energy for water evaporation, has emerged as a promising approach. Graphene oxide (GO)-based membranes possess advantages like capillary action and Marangoni effect, but their stacking defects and dead zones of flexible flakes hinders efficient water transportation, thus the evaporation rate lag behind unobstructed-porous 3D evaporators. Therefore, fundamental mass-transfer approach for optimizing SSG evaporators offers new horizons. Herein, a universal multi-force-fields-based method is presented to regularize membrane channels, which can mechanically eliminate inherent interlayer stackings and defects. Both characterization and simulation demonstrate the effectiveness of this approach across different scales and explain the intrinsic mechanism of mass-transfer enhancement. When combined with a structurally optimized substrate, the 4Laponite@GO-1 achieves evaporation rate of 2.782 kg m-2 h-1 with 94.48% evaporation efficiency, which is comparable with most 3D evaporators. Moreover, the optimized membrane exhibits excellent cycling stability (10 days) and tolerance to extreme conditions (pH 1-14, salinity 1%-15%), verifies the robust structural stability of regularized channels. This optimization strategy provides simple but efficient way to enhance the SSG performance of GO-based membranes, facilitating their extensive application in sustainable water purification technologies.

2.
Angew Chem Int Ed Engl ; 63(18): e202401747, 2024 Apr 24.
Article in English | MEDLINE | ID: mdl-38373179

ABSTRACT

Two-dimensional (2D) materials with high chemical stability have attracted intensive interest in membrane design for the separation of organic solvents. As a novel 2D material, polymeric fullerenes (C60)∞ with distinctive properties are very promising for the development of innovative membranes. In this work, we report the construction of a 2D (C60)∞ nanosheet membrane for organic solvent separation. The pathways of the (C60)∞ nanosheet membrane are constructed by sub-1-nm lateral channels and nanoscale in-plane pores created by the depolymerization of the (C60)∞ nanosheets. Attributing to ordered and shortened transport pathways, the ultrathin porous (C60)∞ membrane is superior in organic solvent separation. The hexane, acetone, and methanol fluxes are up to 1146.3±53, 900.4±41, and 879.5±42 kg ⋅ m-2 ⋅ h-1, respectively, which are up to 130 times higher than those of the state-of-the-art membranes with similar dye rejection. Our findings demonstrate the prospect of 2D (C60)∞ as a promising nanofiltration membrane in the separation of organic solvents from macromolecular compounds such as dyes, drugs, hormones, etc.

3.
Small ; 20(22): e2309253, 2024 May.
Article in English | MEDLINE | ID: mdl-38126674

ABSTRACT

Atomic thick 2D materials hold great potential as building blocks to construct highly permeable membranes, yet the permeability of laminar 2D material membranes is still limited by their irregularity sheep track-like interlayer channels. Herein, a supramolecular-mediated strategy to induce the regular assembly of high-throughput 2D nanofluidic channels based on host-guest interactions is proposed. Inspired by the characteristics of motorways, supramolecular-mediated ultrathin 2D membranes with broad and continuous regular water transport channels are successfully constructed using graphene oxide (GO) as an example. The prepared membrane achieves an ultrahigh water permeability (369.94 LMH bar-1) more than six times higher than that of the original membranes while maintaining dye rejection above 98.5%, which outperforms the reported 2D membranes. Characterization and simulation results show that the introduction of hyaluronate-grafted ß-cyclodextrin not only expands the interlayer channels of GO membranes but also enables the membranes to operate stably under harsh conditions with the help of host-guest interactions. This universal supramolecular assembly strategy provides new opportunities for the preparation of 2D membranes with high separation performance and reliable and stable nanofluidic channels.

4.
ACS Appl Mater Interfaces ; 15(41): 48154-48167, 2023 Oct 18.
Article in English | MEDLINE | ID: mdl-37801365

ABSTRACT

The uncontrolled release of nitrophenol and dye pollutants into water systems is an increasingly serious worldwide concern, and thus efficient wastewater treatment technologies are urgently needed. Herein we report a novel two-dimensional (2D) transition metal carbides and/or nitrides (Ti3C2Tx MXene) membrane modified with silver nanowires (AgNWs) by vacuum assisted filtration technology for the ultrafast nitrophenol catalysis and water purification applications. Regular and controllable membrane transport channels were constructed by stacking Ti3C2Tx MXene nanosheets. Furthermore, the intercalation of AgNWs into the Ti3C2Tx MXene interlayer greatly enlarged the interlayer spacing, resulting in more gaps for fast and selective molecular transport. The optimized Ti3C2Tx MXene@AgNWs (M@A) membrane exhibited a water flux up to ∼191.9 L/(m2 h) while maintaining a high bovine serum albumin (BSA) rejection of ∼95.4%. We emphatically used M@A membranes as efficient catalysts for the reduction of 4-nitrophenol (4-NP), and the results indicated that M@A-12% membrane exhibited the greatest catalytic reduction ability, and recycling utilization. M@A-12% membrane also had an antibacterial rate of more than 99% against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). This work provides a possibility to expand the application of 2D multifunctional M@A membranes in wastewater treatment and pollutant catalytic degradation.


Subject(s)
Biofouling , Environmental Pollutants , Nanowires , Silver/pharmacology , Biofouling/prevention & control , Escherichia coli , Staphylococcus aureus , Titanium/pharmacology , Nitrophenols , Anti-Bacterial Agents/pharmacology , Antifungal Agents , Catalysis , Water
5.
Angew Chem Int Ed Engl ; 62(52): e202311138, 2023 Dec 21.
Article in English | MEDLINE | ID: mdl-37615530

ABSTRACT

The soaring development of industry exacerbates the shortage of fresh water, making drinking water production an urgent demand. Membrane techniques feature the merits of high efficiency, low energy consumption, and easy operation, deemed as the most potential technology to purify water. Recently, a new type of two-dimensional materials, MXenes as the transition metal carbides or nitrides in the shape of nanosheets, have attracted enormous interest in water purification due to their extraordinary properties such as adjustable hydrophilicity, easy processibility, antifouling resistance, mechanical strength, and light-to-heat transformation capability. In pioneering studies, MXene-based membranes have been evaluated in the past decade for drinking water production including the separation of bacteria, dyes, salts, and heavy metals. This review focuses on the recent advancement of MXene-based membranes for drinking water production. A brief introduction of MXenes is given first, followed by descriptions of their unique properties. Then, the preparation methods of MXene membranes are summarized. The various applications of MXene membranes in water treatment and the corresponding separation mechanisms are discussed in detail. Finally, the challenges and prospects of MXene membranes are presented with the hope to provide insightful guidance on the future design and fabrication of high-performance MXene membranes.

6.
Angew Chem Int Ed Engl ; 62(21): e202302997, 2023 May 15.
Article in English | MEDLINE | ID: mdl-36943400

ABSTRACT

Biological ion channels regulate the ion flow across cell membrane via opening or closing of the pores in response to various external stimuli. Replicating the function of high ion gating effects with artificial porous materials has been challenging. Herein, we report that the self-assembled two-dimensional metal-organic framework (MOF) membrane can serve as an excellent nanofluidic platform for smart regulation of ion transport. The MOF membrane with good photothermal performance exhibits extremely high ion gating ratio (up to 104 ), which is among the highest values in MOF membrane nanochannels for light-controlled ion gating reported so far. By repeatedly turning on and off the light, the nanofluidic device shows outstanding stability and reversibility that can be applied in the remote light-switching system. This work may spark promising applications of MOF membrane with variety of stimuli responsive properties in ion sieving, biosensing, and energy conversion.

7.
Article in English | MEDLINE | ID: mdl-36315245

ABSTRACT

Membranes composed of two-dimensional (2D) materials suffer from low stability and structural swelling and are usually restricted to applications in aqueous systems. Among various 2D materials, graphitic phase carbon nitride (GCN, g-C3N4) has shown great application potential owing to its structural tunability. Herein, we develop a coordination-assisted strategy to regulate the GCN layer spacing and chemical environment via copper ion (Cu2+) coordination-assisted intercalation of enantiopure (1S,2S)-(-)-1,2-diphenyl-1,2-ethanediamine (DPE) between GCN nanosheets. The obtained GCN-Cu-DPE membrane is continuous and intact, free of cracks and pinholes, stable under acidic and alkaline conditions, and exhibits water permeability above 215 L m-2 h-1 bar-1 and a high rejection rate to dye molecules. The membrane is amphiphilicity and thus allows both polar solvent (water) and nonpolar solvent (hexane) to freely pass through. Remarkably, the permeation rate is proportional to the viscosity of the solvent. Benefiting from the chiral space between nanosheets, the GCN-Cu-DPE membrane shows selective permeation of aspartic acid racemate in aqueous systems and limonene racemate in the organic phase. Our work demonstrates a general and promising strategy for chiral membrane fabrication toward high-value-added chiral separation, especially in the pharmaceutical industry.

8.
Angew Chem Int Ed Engl ; 59(24): 9751-9756, 2020 06 08.
Article in English | MEDLINE | ID: mdl-32154614

ABSTRACT

The uncontrolled release of antibiotics and pharmaceuticals into the environment is a worldwide increasing problem. Thus, highly efficient treatment technologies for wastewater are urgently needed. In this work, seven kinds of typical antibiotics (including water and alcohol soluble ones) are successfully separated from the corresponding aqueous and ethanolic solutions using highly regular laminated membranes. Our membranes are assembled with 2-4 µm titanium carbide nanosheets. The solvent permeance through such titanium carbide membrane is one order of magnitude higher than that through most polymeric nanofiltration membranes with similar antibiotics rejection. This high flux is due to the regular two-dimensional (2D) structure resulting from the large aspect ratio of titanium carbide nanosheets. Moreover, the electrostatic interaction between the surface terminations and the antibiotics also affects the rejection and enhances the antifouling property. Such 2D titanium carbide membranes further broaden the application scope of laminated materials for separation and purification of high value added drugs in academia and industry.


Subject(s)
Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/isolation & purification , Membranes, Artificial , Nanostructures/chemistry , Nanotechnology/methods , Polymers/chemistry , Time Factors , Titanium/chemistry
9.
Methods Mol Biol ; 1982: 39-59, 2019.
Article in English | MEDLINE | ID: mdl-31172465

ABSTRACT

Determination of the structure of human neutrophil (PMN) flavocytochrome b (Cytb) is a necessary step for the understanding of the structure-function essentials of NADPH oxidase activity. This understanding is crucial for structure-driven therapeutic approaches addressing control of inflammation and infection. Our work on purification and sample preparation of Cytb has facilitated progress toward the goal of structure determination. Here we describe exploiting immunoaffinity purification of Cytb for initial examination of its size and shape by a combination of classical and cryoelectron microscopic (EM) methods. For these evaluations, we used conventional negative-stain transmission electron microscopy (TEM) to examine both detergent-solubilized Cytb as single particles and Cytb in phosphatidylcholine reconstituted membrane vesicles as densely packed random, partially ordered, and subcrystalline arrays. In preliminary trials, we also examined single particles by cryoelectron microscopy (cryoEM) methods. We conclude that Cytb in detergent and reconstituted in membrane is a relatively compact, symmetrical protein of about 100 Å in maximum dimension. The negative stain, preliminary cryoEM, and crude molecular models suggest that the protein is probably a heterotetramer of two p22phox and gp91phox subunits in both detergent micelles and membrane vesicles. This exploratory study also suggests that high-resolution 2D electron microscopic approaches may be accessible to human material collected from single donors.


Subject(s)
Cell Separation/methods , Cytochrome b Group/metabolism , Microscopy, Electron , NADPH Oxidases/metabolism , Neutrophils/metabolism , Neutrophils/ultrastructure , Antibodies, Monoclonal , Biomarkers , Cryoelectron Microscopy , Cytochrome b Group/chemistry , Cytochrome b Group/isolation & purification , Enzyme Stability , Humans , Liposomes/chemistry , Liposomes/metabolism , Liposomes/ultrastructure , Microscopy, Electron/methods , NADPH Oxidases/chemistry , NADPH Oxidases/isolation & purification , Neutrophils/immunology
10.
ChemSusChem ; 12(1): 275-282, 2019 Jan 10.
Article in English | MEDLINE | ID: mdl-30430758

ABSTRACT

Two-dimensional (2D) lamellar membranes consisting of restacked WS2 nanosheets have shown excellent separation properties for water filtration. The stability, antifouling properties, and antibacterial activities of the WS2 laminar membranes were investigated for practical application. We discovered that the separation properties of the WS2 laminar membranes changed slightly after soaking in water for 28 days as well as that of a 45 h-cross-flow filtration, demonstrating an extraordinary operational stability of the WS2 laminar membranes. The remarkable stability is related to the dominant van der Waals interactions between WS2 nanosheets. In addition, the WS2 laminar membranes exhibited excellent antibacterial properties against S. aureus and E. coli with antibacterial rates of 91.3 % and 89.7 %, respectively. These properties of the WS2 laminar membranes make them promising candidates for application in water filtration.

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