Per- and polyfluoroalkyl substances (PFAS) have been extensively utilized in practical applications that include surfactants, lubricants, and firefighting foams due to their thermal stability and chemical inertness. Recent studies have revealed that PFAS were detected in groundwater and even drinking water systems which can cause severe environmental and health issues. While adsorbents with a large specific surface area have demonstrated effective removal of PFAS from water, their capability in desorbing the retained PFAS has been often neglected despite its critical role in regeneration for reuse. Further, they have demonstrated a relatively lower adsorption capacity for PFAS with a short fluoroalkyl chain length. To overcome these limitations, electric field-aided adsorption has been explored. In this work, reversible adsorption and desorption of PFAS dissolved in water upon alternating voltage is reported. An inexpensive graphite adsorbent is fabricated by using a simple press resulting in a mesoporous structure with a BET surface area of 132.9 ± 10.0 m2 g−1. Electric field-aided adsorption and desorption experiments are conducted by using a custom-made cell consisting of two graphite electrodes placed in parallel in a polydimethylsiloxane container. Unlike the conventional sorption process, a graphite electrode exhibits a higher adsorption capacity for PFAS with a short fluoroalkyl chain (perfluoropentanoic acid, PFPA) in comparison to that with a long fluoroalkyl chain (perfluorooctanoic acid, PFOA). Upon alternating the voltage to a negative value, the retained PFPA or PFOA is released into the surrounding water. Finally, we engineered a device module mounted on a gravity-assisted apparatus to demonstrate electrosorption of PFAS and collection of high purity water.
8 February 2024 in ACS Applied Engineering Materials
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.
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.
Superomniphobic surfaces that can self-repair physical damage are desirable for sustainable performance over time in many practical applications that include self-cleaning, corrosion resistance, and protective gears. However, fabricating such self-repairing superomniphobic surfaces has thus far been a challenge because it necessitates the regeneration of both low-surface-energy materials and hierarchical topography. Herein, a water-responsive self-repairing superomniphobic film is reported by utilizing cross-linked hydroxypropyl cellulose (HPC) composited with silica (SiO2) nanoparticles (HPC-SiO2) that is treated with a low-surface-energy perfluorosilane. The film can repair physical damage (e.g., a scratch) in approximately 10 s by regenerating its hierarchical topography and low-surface-energy material upon the application of water vapor. The repaired region shows an almost complete recovery of its inherent superomniphobic wettability and mechanical hardness. The repairing process is driven by the reversible hydrogen bond between the hydroxyl (−OH) groups which can be dissociated upon exposure to water vapor. This results in a viscous flow of the HPC-SiO2 film into the damaged region. A mathematical model composed of viscosity and surface tension of the HPC-SiO2 film can describe the experimentally measured viscous flow with reasonable accuracy. Finally, we demonstrate that the superomniphobic HPC-SiO2 film can repair physical damage by a water droplet pinned on a damaged area or by sequential rolling water droplets.