Award Abstract # 1605088
Collaborative Research: Coupled effects of particle shape/flexibility and pore morphology on membrane rejection: theory and experiment

NSF Org: CBET
Division of Chemical, Bioengineering, Environmental, and Transport Systems
Recipient: TEXAS A&M ENGINEERING EXPERIMENT STATION
Initial Amendment Date: July 14, 2016
Latest Amendment Date: June 30, 2021
Award Number: 1605088
Award Instrument: Standard Grant
Program Manager: Christina Payne
cpayne@nsf.gov
 (703)292-2895
CBET
 Division of Chemical, Bioengineering, Environmental, and Transport Systems
ENG
 Directorate for Engineering
Start Date: August 15, 2016
End Date: July 31, 2022 (Estimated)
Total Intended Award Amount: $160,155.00
Total Awarded Amount to Date: $172,155.00
Funds Obligated to Date: FY 2016 = $160,155.00
FY 2017 = $6,000.00

FY 2021 = $6,000.00
History of Investigator:
  • Shankar Chellam (Principal Investigator)
    chellam@tamu.edu
Recipient Sponsored Research Office: Texas A&M Engineering Experiment Station
3124 TAMU
COLLEGE STATION
TX  US  77843-3124
(979)862-6777
Sponsor Congressional District: 10
Primary Place of Performance: Texas A&M Engineering Experiment Station
3136 TAMU
College Station
TX  US  77843-3136
Primary Place of Performance
Congressional District:
10
Unique Entity Identifier (UEI): QD1MX6N5YTN4
Parent UEI: QD1MX6N5YTN4
NSF Program(s): Interfacial Engineering Progra
Primary Program Source: 01001617DB NSF RESEARCH & RELATED ACTIVIT
01001718DB NSF RESEARCH & RELATED ACTIVIT

01002122DB NSF RESEARCH & RELATED ACTIVIT
Program Reference Code(s): 9251
Program Element Code(s): 141700
Award Agency Code: 4900
Fund Agency Code: 4900
Assistance Listing Number(s): 47.041

ABSTRACT

Proposal Numbers: 1604715 (Lead)/1605088 PIs: Baltus, R.E./Chellam, S.
Collaborative Research: Coupled effects of particle shape/flexibility and pore morphology on membrane rejection: theory and experiment

The motivation for this research lies in the fact that by the year 2025, nearly 2 billion people are projected to live in areas of water scarcity. These drivers point to the need for advanced water and wastewater treatment technologies to alleviate ever-increasing water demand. Low-pressure liquid-solid membrane separation technologies such as microfiltration and ultrafiltration directly remove difficult-to disinfect parasites such as Giardia and Cryptosporidium, along with most bacteria, turbidity, and other colloidal materials. However, micro- and ultrafilters are not effective in removing viruses and some bacteria. The overall goal of this research is to examine the impact of non-ideal pore geometry and particle shape and flexibility on microbial rejection by porous membranes. This collaborative research project will perform both mathematical modeling and experimental work to quantitatively examine complex systems that more closely represent real-world separations. Results generated from this project will be important for the optimal design of micro- and ultrafiltration systems and for practical applications related to water and wastewater treatment and food, biotechnological, and pharmaceutical operations. Educational broader impacts include the development of science outreach activities geared towards elementary, middle, and high schools in neighboring communities in College Station, TX and Potsdam, NY to attract underrepresented minorities into STEM fields.

Currently available membrane system design strategies are based on simple pore geometries and microbial shapes. Consequently, they cannot fully explain incomplete microbial removal observed in practice. This collaborative project will generate fundamental knowledge to characterize the hindered convection of tailed viruses, filamentous viruses, deformable bacteria, and rigid synthetic nanorods across porous membranes with tortuous interconnected pore networks. The project tightly integrates the experimental and theoretical efforts. The project will focus on separations of tailed and flexible viral and bacterial particles using low-pressure membranes with capillary pores as well as membrane systems with complex pore morphology. One example of the technological impact of this research is that it is addressing the difficulty in removing tailed viruses that are among the most abundant organisms in the environment and have been shown to penetrate so-called sterile filters. The research will examine whether flexible particles will be able to navigate around pore bends and whether bacteria that lack rigid cell walls can squeeze through pores. To theoretically examine particle shape and flexibility, detailed models of particle transport in a single cylindrical pore will be developed. Specifically, the physics of the non-spherical shape and flexibility of the viruses and bacteria will be incorporated. Experiments to validate these model predictions will be performed using track-etched membranes. To examine effects of membrane morphology including pore interconnectivity, 2D permeation measurements will be performed and interpreted using models developed to describe these systems. This project will generate a quantitative understanding of the role of complex pore geometries and microbial characteristics that govern rejection of microorganism from porous membranes. Incorporating such considerations will improve existing filtration models to more accurately describe rejection in real-world membrane separations.

PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH

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Kyungho Kim, Anindito Sen, and Shankararaman Chellam "Removal and inactivation of non-enveloped and enveloped virus surrogates by conventional coagulation and electrocoagulation using aluminum and iron" Journal , v.2 , 2022 , p.1974 https://doi.org/10.1021/acsestengg.2c00128
Kyungho Kim, Jothikumar Narayanan, Anindito Sen, and Shankararaman Chellam "Virus Removal and Inactivation Mechanisms during Iron Electrocoagulation: Capsid and Genome Damages and Electro-Fenton Reactions" Journal , v.55 , 2021 , p.13198 https://doi.org/10.1021/acs.est.0c04438
Kyungho Kim, Jothikumar Narayanan, Anindito Sen, Jennifer L. Murphy, and Shankararaman Chellam "Removal and Inactivation of an Enveloped Virus Surrogate by Iron Conventional Coagulation and Electrocoagulation" Environmental Science and Technology , v.55 , 2021 , p.2674 https://dx.doi.org/10.1021/acs.est.0c07697
R.E. Baltus, A.R. Badireddy, A. Delavari, and S. Chellam "Free Diffusivity of Icosahedral and Tailed Bacteriophages: Experiments, Modeling, and Implications for Virus Behavior in Media Filtration and Flocculation" Environmental Science & Technology , v.51 , 2017 , p.1433 10.1021/acs.est.6b05323

PROJECT OUTCOMES REPORT

Disclaimer

This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.

The overarching focus of this project was microorganism control in drinking water.  To accomplish this a two-pronged approach was taken: (1) virus attenuation by processes currently implemented in water treatment plants and novel promising technologies and (2) bacterial removal by microfiltration.

First, we considered two structural types of viruses: those that have an outer fortress, called an envelope, and those that do not since both are present in wastewater.  Using a coronavirus surrogate, we presented strong evidence that existing water treatment facilities can easily reduce vast quantities of enveloped viruses, thereby protecting household water from such contagions.  In particular, the water purification step called coagulation could alone get rid of 99.999% of the virus, markedly decontaminating water for consumption.  For these experiments, a known concentration of coronavirus surrogate was added to clean water.  Next, we tested the action of coagulants commonly used in water treatment plants.  After coagulation, we examined small samples of the virus-infused water under an electron microscope and found that the virus strain assembled on the coagulants, forming clusters.  We then checked the presence of infectious viruses in the water after removing the clumps and found a tremendous reduction.

Next, using sophisticated microscopy and computational analysis, we validated the merit of a water purification technology that uses electricity to remove and inactivate an assortment of waterborne viruses.  This novel water purification technology is called electrocoagulation, which could add another level of safety against pathogens that cause gastrointestinal ailments and other infections in humans.  Conventional coagulation methods use chemicals to trigger the clumping of particles and microbes within untreated water.  These aggregates can then be removed when they settle as sediments.  While effective, coagulation chemicals could be very acidic, making their transport to treatment plants and storage a challenge.  Instead of chemicals-based coagulation, we investigated if an up-and-coming coagulation method that uses electricity was as effective at removing microbes from water.

For these experiments, iron or aluminum electrodes were inserted in a sample of untreated water laden with viruses.  When electrical current was passed, the anode oxidized, releasing iron and aluminum ions into the solution.  In the process, as aluminum and iron precipitated, viruses attached to these clumps to form bigger aggregates, which were easily removed from the water.  Iron outperformed aluminum because it was able to combine with dissolved oxygen to produce hydroxyl radicals, which chemically reacted with viruses thereby inactivating them (a process that did not occur with aluminum).  An important contribution of our research was that we pictured viral inactivation using electron microscopy.

Clumping caused a tremendous challenge because there is no easy way to isolate the virus from the metal-rich aggregates, making it difficult to visualize viral damage and analyze if iron electrocoagulation was the cause of the viral damage or the virus extraction from the iron-rich clumps.  To address this problem, we developed a novel computational technique to directly image the viruses aggregated alongside iron/aluminum.  We found that iron electrocoagulated non-enveloped viruses were significantly damaged but not those isolated from conventional coagulation.  In contrast, both conventional coagulation and electrocoagulation and both iron and aluminum coagulants damaged enveloped viruses.  Iron electrocoagulation concurrently removed and inactivated viruses to achieve equivalent or higher total reductions with less charge consumption compared with aluminum suggesting its superiority as a water purification process.

Traditionally, water purification is a multistep process to ensure that even if one step fails, the subsequent ones can ensure safety - a multiple barrier approach, so to speak.  In this research, we presented evidence that process intensification with electrocoagulation, where coagulation and disinfection are combined within a single step before subsequent purification stages, ensured better protection against waterborne pathogens.

Finally, we investigated bacterial removal by microfiltration and the ability of bacteria to clog filters.  We selected a bacterium lacking cell walls, which rendered them deformable under typical filtration pressures.  Specifically, we evaluated the behavior of Acholeplasma laidlawii by microfiltration membranes.  This bacterium even passed through so-called ?sterile filters? (rated at 100 nanometers) thereby representing a new worst-case scenario to test membrane rejection and their ability to sterilize feed streams of biotechnological importance.  Additionally, in comparison with rigid silica particles of the same size under identical testing conditions, these ?squishy? bacteria clogged filters to a significantly greater extent by compressing against their surface and restricted flow.

Further, parallel to laboratory experiments and computational modeling, we designed several water purification lesson plans aimed at elementary and high school students.  Undergraduate students were trained to demonstrate these experiments on multiple occasions at local K-12 schools.  We also participated in "career days" at a rural school to convey the importance of pursuing a STEM education and the benefits of engineering careers.


Last Modified: 11/23/2022
Modified by: Shankar Chellam

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