Bacterial Cellulose Spheres that Encapsulate Solid Materials.

Bacterial cellulose (BC) spheres have been increasingly researched since the popularization of BC as a novel material. This protocol presents an affordable and simple method for BC sphere production. In addition to producing these spheres, an encapsulation method for solid particles has also been identified. To produce BC spheres, water, black tea, sugar, vinegar, and bacterial culture are combined in a baffled flask and the contents are agitated. After determining the proper culture conditions for BC sphere formation, their ability to encapsulate solid particles was tested using biochar, polymer beads, and mine waste. Spheres were characterized using ImageJ software and thermal gravimetric analysis (TGA). Results indicate that spheres with 7.5 mm diameters can be made in 7 days. Adding various particles increases the average size range of the BC capsules. The spheres encapsulated 10 - 20% of their dry mass. This method shows low-cost sphere production and encapsulation that is possible with easily obtainable materials. BC spheres may be used in the future as a contaminant removal aid, controlled release fertilizer coating, or soil amendment.

Quantification and modeling of the response of surface biofilm growth to continuous low intensity UVC irradiation.

Though germicidal UV radiation is widely applied for disinfection of water and food, it may also be used to prevent bacterial growth and colonization on surfaces within engineered systems. Emerging UV source technologies, such as ultraviolet-C (UVC) LEDs, present new opportunities for deterring biofilms within certain devices, including medical equipment, food equipment, and potentially in plumbing fixtures for prevention of opportunistic respiratory pathogen infections. Rational design for incorporation of UVC sources into devices with complex internal geometries is currently hampered by the lack of an engineering framework for predicting reductions in biofilm growth rates in response to continuous low-intensity irradiation. Herein we have developed an experimental apparatus and method for growing biofilms under concurrent UV irradiation and quantifying the resulting suppression of surface growth. Under accelerated growth conditions over 48 h, E. coli surface biovolume was reduced by 95% compared to control biofilms (grown in the dark) by a UV intensity of 50.5 µW/cm2 (254 nm). The required intensity for biofilm prevention was higher than expected, given the UV dose response of the bacteria employed and the cumulative doses delivered to the test surfaces. The results indicate that biofilms can establish even under irradiation conditions that would result in complete inactivation of planktonic cells, likely due to the shielding effects of colloidal material and microbial exudates. A pseudo-mechanistic model was also developed which correlated UV intensity to the resultant reduction in specific surface biovolume.

Facile Postprocessing Alters the Permeability and Selectivity of Microbial Cellulose Ultrafiltration Membranes.

Water filtration membranes produced sustainably through microbial cellulose production can have filtration properties altered through facile chemical treatments. Microbial cellulose is an effective membrane filtration medium, and pristine microbial membranes can serve as ultrafiltration membranes with a permeability of 143 L m-2h-1bar-1 and a particle size cut off of 35 nm. As living biofilms, these membranes consist of microbial cellulose, bacteria, and extracellular polymers. Thus, additional biofilm components may reduce the intrinsic permeability of the cellulose. Here, microbial membranes were treated with hydrogen peroxide (H2O2) and sodium hypochlorite (NaOCl, liquid bleach) to remove impurities present in microbial cellulose and increase membrane permeability. For example, permeability increased from 143 to 257 L m-2h-1bar-1 with treatment by 0.3% H2O2 for 12 min. The membranes were also treated with sodium hydroxide (NaOH) to increase membrane selectivity, and the particle size cutoff was reduced from 35 to 10 nm post-treatment with 0.8% NaOH for 20 min. Scanning electron microscopy, Fourier-transform infrared spectroscopy, thermogravimetric analysis, contact angle goniometry, and X-ray diffraction were used to characterize the physical and chemical properties of the membrane matrix. Facile chemical treatments provide a significant degree of flexibility to tailor microbial membranes to meet specific needs. Microbial membrane production is inherently accessible, and this study furthers that accessibility by utilizing only readily available components to treat microbial membranes and expand their potential applications.

Permeability is the Critical Factor Governing the Life Cycle Environmental Performance of Drinking Water Treatment Using Living Filtration Membranes.

Living Filtration Membranes (LFMs) are a water filtration technology that was recently developed in the lab (Technology Readiness Level 4). LFMs have shown filtration performance comparable with that of ultrafiltration, far better fouling resistance than conventional polymer membranes, and good healing capabilities. These properties give LFMs promise to address two significant issues in conventional membrane filtration: fouling and membrane damage. To integrate environmental considerations into future technology development (i.e., Ecodesign), this study assesses the life cycle environmental performance of drinking water treatment using LFMs under likely design and operation conditions. It also quantitatively ranks the engineering design and operation factors governing the further optimization of LFM environmental performance using a global sensitivity analysis. The results suggest that LFMs' superior fouling resistance will reduce the life cycle environmental impacts of ultrafiltration by 25% compared to those of a conventional polymer membrane in most impact categories (e.g., acidification, global warming potential, and carcinogenics). The only exception is the eutrophication impact, where the need for growth medium and membrane regeneration offsets the benefits of LFMs' fouling resistance. Permeability is the most important factor that should be prioritized in future R&D to further improve the life cycle environmental performance of LFMs. A 1% improvement in the permeability will lead to a ∼0.7% improvement in LFMs' environmental performance in all the impact categories, whereas the same change in the other parameters investigated (e.g., LFM lifespan and regeneration frequency) typically only leads to a <0.2% improvement.

Sustainable Living Filtration Membranes.

As demand for clean water increases, there is a growing need for effective sustainable water treatment systems. We used the symbiotic culture of bacteria and yeast (SCOBY) that forms while brewing kombucha tea as a living water filtration membrane (LFM). The LFMs function as ultrafiltration membranes with a permeability of 135 ± 25 L m-2 h-1 bar-1 and a 90% rejection of 30 nm nanoparticles. Because they contain living microorganisms that produce cellulose fibers, the surface of an LFM heals after a puncture or incision. Following punctures or incisions, membrane permeability, after a rapid increase postpuncture, returns to 110-250% of the original flux after 10 days in a growth solution. Additionally, LFMs may be manufactured using readily available materials, increasing membrane production accessibility.

Acid Rock Drainage Treatment Using Membrane Distillation: Impacts of Chemical-Free Pretreatment on Scale Formation, Pore Wetting, and Product Water Quality.

Acid rock drainage (ARD) is a metal-rich wastewater that forms upon oxidation of sulfidic minerals. Although ARD impacts >12,000 miles of rivers in the U.S. and has an estimated cleanup cost of $32-$72 billion, the low pH and high metal concentrations in ARD make rapid, high volume treatment without chemical addition difficult. This research focuses on a novel method of ARD treatment, membrane distillation (MD). In MD, heated ARD is separated from a cooled distillate by a hydrophobic, water-excluding membrane. Because water only passes through the membrane in the vapor phase, nonvolatile sulfate and heavy metals are retained in the concentrate stream. A preliminary in silico analysis using an electrolyte thermodynamic model indicated that MD of 10 different mine wastes yields product water containing no contaminants at concentrations >0.2 ppm. MD tests of synthetic ARD used a ∼34 °C temperature difference, operated at 80% recovery, and produced an initial flux of 38.4 ± 1.1 L·m-2·h-1. This flux decreased slightly after scaling by iron oxyhydroxide; however, membranes maintained >99% dissolved solids rejection. Both flux decline and membrane scale formation decreased after a chemical-free, thermal precipitation pretreatment. These results indicate that MD can purify contaminated, acidic wastewater using low-grade heat sources, such as geothermal energy, without chemical addition.

Advanced Materials, Technologies, and Complex Systems Analyses: Emerging Opportunities to Enhance Urban Water Security.

Innovation in urban water systems is required to address the increasing demand for clean water due to population growth and aggravated water stress caused by water pollution, aging infrastructure, and climate change. Advances in materials science, modular water treatment technologies, and complex systems analyses, coupled with the drive to minimize the energy and environmental footprints of cities, provide new opportunities to ensure a resilient and safe water supply. We present a vision for enhancing efficiency and resiliency of urban water systems and discuss approaches and research needs for overcoming associated implementation challenges.

Nanophotonics-enabled solar membrane distillation for off-grid water purification.

With more than a billion people lacking accessible drinking water, there is a critical need to convert nonpotable sources such as seawater to water suitable for human use. However, energy requirements of desalination plants account for half their operating costs, so alternative, lower energy approaches are equally critical. Membrane distillation (MD) has shown potential due to its low operating temperature and pressure requirements, but the requirement of heating the input water makes it energy intensive. Here, we demonstrate nanophotonics-enabled solar membrane distillation (NESMD), where highly localized photothermal heating induced by solar illumination alone drives the distillation process, entirely eliminating the requirement of heating the input water. Unlike MD, NESMD can be scaled to larger systems and shows increased efficiencies with decreased input flow velocities. Along with its increased efficiency at higher ambient temperatures, these properties all point to NESMD as a promising solution for household- or community-scale desalination.

Biofouling and microbial communities in membrane distillation and reverse osmosis.

Membrane distillation (MD) is an emerging desalination technology that uses low-grade heat to drive water vapor across a microporous hydrophobic membrane. Currently, little is known about the biofilms that grow on MD membranes. In this study, we use estuarine water collected from Long Island Sound in a bench-scale direct contact MD system to investigate the initial stages of biofilm formation. For comparison, we studied biofilm formation in a bench-scale reverse osmosis (RO) system using the same feedwater. These two membrane desalination systems expose the natural microbial community to vastly different environmental conditions: high temperatures with no hydraulic pressure in MD and low temperature with hydraulic pressure in RO. Over the course of 4 days, we observed a steady decline in bacteria concentration (nearly 2 orders of magnitude) in the MD feed reservoir. Even with this drop in planktonic bacteria, significant biofilm formation was observed. Biofilm morphologies on MD and RO membranes were markedly different. MD membrane biofilms were heterogeneous and contained several colonies, while RO membrane biofilms, although thicker, were a homogeneous mat. Phylogenetic analysis using next-generation sequencing of 16S rDNA showed significant shifts in the microbial communities. Bacteria representing the orders Burkholderiales, Rhodobacterales, and Flavobacteriales were most abundant in the MD biofilms. On the basis of the results, we propose two different regimes for microbial community shifts and biofilm development in RO and MD systems.

In situ formation of silver nanoparticles on thin-film composite reverse osmosis membranes for biofouling mitigation.

The potential to incorporate silver nanoparticles (Ag-NPs) as biocides in membranes for water purification has gained much interest in recent years. However, a viable strategy for loading the Ag-NPs on the membrane remains challenging. This paper presents a novel, facile procedure for loading Ag-NPs on thin-film composite (TFC) reverse osmosis membranes. Reaction of silver salt with a reducing agent on the membrane surface resulted in uniform coverage of Ag-NPs, irreversibly bound to the membrane, as confirmed by XPS, TEM, and SEM analyses. Salt selectivity of the membrane as well its surface roughness, hydrophilicity, and zeta potential were not impacted by Ag-NP functionalization, while a slight reduction (up to 17%) in water permeability was observed. The formed Ag-NPs imparted strong antibacterial activity to the membrane, leading to reduction of more than 75% in the number of live bacteria attached to the membrane for three model bacteria strains. In addition, confocal microscopy analyses revealed that Ag-NPs significantly suppressed biofilm formation, with 41% reduction in total biovolume and significant reduction in EPS, dead, and live bacteria on the functionalized membrane. The simplicity of the method, the short reaction time, the ability to load the Ag-NPs on site, and the strong imparted antibacterial activity highlight the potential of this method in real-world RO membrane applications.

Surface functionalization of thin-film composite membranes with copper nanoparticles for antimicrobial surface properties.

Biofouling is a major operational challenge in reverse osmosis (RO) desalination, motivating a search for improved biofouling control strategies. Copper, long known for its antibacterial activity and relatively low cost, is an attractive potential biocidal agent. In this paper, we present a method for loading copper nanoparticles (Cu-NPs) on the surface of a thin-film composite (TFC) polyamide RO membrane. Cu-NPs were synthesized using polyethyleneimine (PEI) as a capping agent, resulting in particles with an average radius of 34 nm and a copper content between 39 and 49 wt.%. The positive charge of the Cu-NPs imparted by the PEI allowed a simple electrostatic functionalization of the negatively charged RO membrane. We confirmed functionalization and irreversible binding of the Cu-NPs to the membrane surface with SEM and XPS after exposing the membrane to bath sonication. We also demonstrated that Cu-NP functionalization can be repeated after the Cu-NPs dissolve from the membrane surface. The Cu-NP functionalization had minimal impact on the intrinsic membrane transport parameters. Surface hydrophilicity and surface roughness were also maintained, and the membrane surface charge became positive after functionalization. The functionalized membrane exhibited significant antibacterial activity, leading to an 80-95% reduction in the number of attached live bacteria for three different model bacterial strains. Challenges associated with this functionalization method and its implementation in RO desalination are discussed.

Biodegradable polymer (PLGA) coatings featuring cinnamaldehyde and carvacrol mitigate biofilm formation.

Biofilm-associated infections are one of the leading causes of death in the United States. Although infections may be treated with antibiotics, the overuse of antibiotics has led to the spread of antibiotic resistance. Many natural antimicrobial compounds derived from edible plants are safe for human use and target bacteria nonspecifically. Therefore, they may impair biofilm formation with less evolutionary pressure on pathogens. Here, we explore the use of two natural antimicrobial compounds, cinnamaldehyde (CA, from cinnamon) and carvacrol (CARV, from oregano), for biofilm prevention. We have fabricated and characterized films that incorporate CA and CARV into the biodegradable, FDA-approved polymer poly(lactic-co-glycolic acid), PLGA. The addition of CA and CARV to PLGA films not only adds antimicrobial activity but also changes the surface properties of the films, making them more hydrophilic and therefore more resistant to bacterial attachment. An addition of 0.1% CA to a PLGA film significantly impairs biofilm development by Staphylococcus aureus, and 0.1% CARV in PLGA significantly decreases biofilm formation by both Escherichia coli and S. aureus. Pseudomonas aeruginosa, which is less susceptible to CA and CARV, was not affected by the addition of 0.1% CA or CARV to the PLGA coatings; however, P. aeruginosa biofilm was significantly reduced by 1.0% CA. These results indicate that both CA and CARV could potentially be used in low concentrations as natural additives in polymer coatings for indwelling devices to delay colonization by bacteria.

Electronic-structure-dependent bacterial cytotoxicity of single-walled carbon nanotubes.

Single-walled carbon nanotubes (SWNTs) have been previously observed to be strong antimicrobial agents, and SWNT coatings can significantly reduce biofilm formation. However, the SWNT antimicrobial mechanism is not fully understood. Previous studies on SWNT cytotoxicity have concluded that membrane stress (i.e., direct SWNT-bacteria contact resulting in membrane perturbation and the release of intracellular contents) was the primary cause of cell death. Gene expression studies have indicated oxidative stress may be active, as well. Here, it is demonstrated for the first time how SWNT electronic structure (i.e., metallic versus semiconducting) is a key factor regulating SWNT antimicrobial activity. Experiments were performed with well-characterized SWNTs of similar length and diameter but varying fraction of metallic nanotubes. Loss of Escherichia coli viability was observed to increase with an increasing fraction of metallic SWNTs. Time-dependent cytotoxicity measurements indicated that in all cases the majority of the SWNT antimicrobial action occurs shortly after (<15 min) bacteria-SWNT contact. The SWNT toxicity mechanism was investigated by in vitro SWNT-mediated oxidation of glutathione, a common intracellular thiol that serves as an antioxidant and redox state mediator. The extent of glutathione oxidation was observed to increase with increasing fraction of metallic SWNTs, indicating an elevated role of oxidative stress. Scanning electron microscopy images of E. coli in contact with the SWNTs demonstrated electronic structure-dependent morphological changes consistent with cytotoxicity and glutathione oxidation results. A three-step SWNT antimicrobial mechanism is proposed involving (i) initial SWNT-bacteria contact, (ii) perturbation of the cell membrane, and (iii) electronic structure-dependent bacterial oxidation.