Membrane-based separation technologies are attractive to remediating unconventional water sources, including brackish, industrial, and municipal wastewater, due to their versatility and relatively high energy efficiency. However, membrane fouling by dissolved or suspended organic substances remains a primary challenge which can result in an irreversible decline of the permeate flux. To overcome this, membranes have been incorporated with photocatalytic materials that can degrade these organic substances deposited on the surface upon light illumination. While such photocatalytic membranes have demonstrated that they can recover their inherent permeability, less information is known about the effect of photocatalysis on the kinetics of the permeate flux. In this work, a photocatalytic mesh that can selectively permeate water while repelling oil was fabricated by coating a mixture of nitrogen-doped TiO2(N-TiO2) and perfluorosilane-grafted SiO2(F-SiO2) nanoparticles on a stainless steel mesh. Utilizing the photocatalytic mesh, the time-dependent evolution of the water-rich permeate flux as a result of photocatalytic degradation of the oil was studied under the visible light illumination. A mathematical model was developed that can relate the photocatalytic degradation of the organic substances deposited on a mesh surface to the evolution of the permeate flux. This model was established by integrating the Langmuir–Hinshelwood kinetics for photocatalysis and the Cassie–Baxter wettability analysis on a chemically heterogeneous mesh surface into a permeate flux relation. Consequently, the time-dependent water-rich permeate flux values are compared with those predicted by using the model. It is found that the model can predict the evolution of the water-rich permeate flux with a goodness of fit of 0.92.
Selective Wettability Membrane for Continuous Oil−Water Separation and In Situ Visible Light‐Driven Photocatalytic Purification of Water
Membrane‐based technologies are attractive for remediating oily wastewater because they are relatively energy‐efficient and are applicable to a wide range of industrial effluents. For complete treatment of oily wastewater, removing dissolved contaminants from the water phase is typically followed by adsorption onto an adsorbent, which complicates the process. Here, an in‐air superhydrophilic and underwater superoleophobic membrane‐based continuous separation of surfactant‐stabilized oil‐in‐water emulsions and in situ decontamination of water by visible‐light‐driven photocatalytic degradation of dissolved organic contaminants is reported. The membrane is fabricated by utilizing a thermally sensitized stainless steel mesh coated with visible light absorbing iron‐doped titania nanoparticles. Post annealing of the membrane can enhance the adhesion of nanoparticles to the membrane surface by formation of a bridge between them. An apparatus that enables continuous separation of surfactant‐stabilized oil‐in‐water emulsion and in situ photocatalytic degradation of dissolved organic matter in the water‐rich permeate upon irradiation of visible light on the membrane surface with greater than 99% photocatalytic degradation is developed. The membrane demonstrates the recovery of its intrinsic water‐rich permeate flux upon continuous irradiation of light after being contaminated with oil. Finally, continuous oil−water separation and in situ water decontamination is demonstrated by photocatalytically degrading model toxins in water‐rich permeate.
more » « less- Award ID(s):
- 1801710
- NSF-PAR ID:
- 10456516
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Global Challenges
- Volume:
- 4
- Issue:
- 10
- ISSN:
- 2056-6646
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
Membrane-based separation technologies are the cornerstone of remediating unconventional water sources, including brackish and industrial or municipal wastewater, as they are relatively energy-efficient and versatile. However, membrane fouling by dissolved and suspended substances in the feed stream remains a primary challenge that currently prevents these membranes from being used in real practices. Thus, we directly address this challenge by applying a superhydrophilic and oleophobic coating to a commercial membrane surface which can be utilized to separate and desalinate an oil and saline water mixture, in addition to photocatalytically degrading the organic substances. We fabricated the photocatalytic membrane by coating a commercial membrane with an ultraviolet (UV) light-curable adhesive. Then, we sprayed it with a mixture of photocatalytic nitrogen-doped titania (N-TiO2) and perfluoro silane-grafted silica (F-SiO2) nanoparticles. The membrane was placed under a UV light, which resulted in a chemically heterogeneous surface with intercalating high and low surface energy regions (i.e., N-TiO2 and F-SiO2, respectively) that were securely bound to the commercial membrane surface. We demonstrated that the coated membrane could be utilized for continuous separation and desalination of an oil–saline water mixture and for simultaneous photocatalytic degradation of the organic substances adsorbed on the membrane surface upon visible light irradiation.more » « less
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null (Ed.)The recalcitrance of some emerging organic contaminants through conventional water treatment systems may necessitate advanced technologies that use highly reactive, non-specific hydroxyl radicals. Here, polyacrylonitrile (PAN) nanofibers with embedded titanium dioxide (TiO 2 ) nanoparticles were synthesized via electrospinning and subsequently carbonized to produce mechanically stable carbon/TiO 2 (C/TiO 2 ) nanofiber composite filters. Nanofiber composites were optimized for reactivity in flow through treatment systems by varying their mass loading of TiO 2 , adding phthalic acid (PTA) as a dispersing agent for nanoparticles in electrospinning sol gels, comparing different types of commercially available TiO 2 nanoparticles (Aeroxide® P25 and 5 nm anatase nanoparticles) and through functionalization with gold (Au/TiO 2 ) as a co-catalyst. High bulk and surface TiO 2 concentrations correspond with enhanced nanofiber reactivity, while PTA as a dispersant makes it possible to fabricate materials at very high P25 loadings (∼80% wt%). The optimal composite formulation (50 wt% P25 with 2.5 wt% PTA) combining high reactivity and material stability was then tested across a range of variables relevant to filtration applications including filter thickness (300–1800 μm), permeate flux (from 540–2700 L m −2 h), incident light energy (UV-254 and simulated sunlight), flow configuration (dead-end and cross-flow filtration), presence of potentially interfering co-solutes (dissolved organic matter and carbonate alkalinity), and across a suite of eight organic micropollutants (atrazine, benzotriazole, caffeine, carbamazepine, DEET, metoprolol, naproxen, and sulfamethoxazole). During cross-flow recirculation under UV-irradiation, 300 μm thick filters (30 mg total mass) produced micropollutant half-lives ∼45 min, with 40–90% removal (from an initial 0.5 μM concentration) in a single pass through the filter. The initial reaction rate coefficients of micropollutant transformation did not clearly correlate with reported second order rate coefficients for reaction with hydroxyl radical ( k OH ), implying that processes other than reaction with photogenerated hydroxyl radical ( e.g. , surface sorption) may control the overall rate of transformation. The materials developed herein represent a promising next-generation filtration technology that integrates photocatalytic activity in a robust platform for nanomaterial-enabled water treatment.more » « less
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