Assessing the risks of manufactured nanomaterials.
Explore the source record for details and available documents.
Animals↗
Biomedical subjects
Pratim Biswas
Publications and source records attributed to Pratim Biswas.
Charge reduced electrospray size spectrometry of mega- and gigadalton complexes: whole viruses and virus fragments.
The ability to analyze and identify large macromolecular complexes whose molecular weight is beyond the analyzable range of mass spectrometry is of great interest. The size of such complexes makes them suitable for analysis via mobility size spectrometry. In this work, charge reduced electrospray size spectrometry was used for the analysis of bacteriophage viruses with total molecular masses ranging from 3.6 MDa up to the gigadalton range. The electrospray source used was operated in "cone jet" mode with a mean droplet diameter of 170.56 nm. Bacteriophage MS2 was found to have a mobility diameter of 24.13 +/- 0.06 nm and remain highly viable after the electrospray process. Larger bacteriophages T2 and T4 have lengths greater than the diameter of the electrospray jet and droplets; thus, they could not be completely enclosed and were found to fragment at the virus capsid head-tail noncovalent interface during either the jet formation or jet breakup process. No viable T2 or T4 virions were detectable after being electrosprayed. While the exact mechanism of fragmentation could not be determined, it is proposed here that macromolecular fragmentation at noncovalent interfaces occurs due to mechanically and electrically induced stresses during jet formation and jet breakup. Bacteriophage T4 capsid heads were found to be statistically significantly larger than bacteriophage T2 capsid heads, with a mean peak diameter of 88.32 +/- 1.02 nm for T4 and 87.03 +/- 0.18 nm for T2. While capsid head fragments were detectable, tail and tail-fiber fragments could not be detected by size spectrometric analysis. This is attributed to the fact that the contractile tails of bacteriophage T2 and T4 virions mechanically deform to a varying degree while confined within the smaller jet and droplets. Further evidence of contractile tail deformation during the electrospray process was found by measuring the size spectrum of bacteriophage lambda, which has a noncontractile tail. Bacteriophage lambda had two distinct peaks in its size spectrum, one corresponding to the capsid head and the other corresponding to the tail fragment. Size spectrometry was also used for rapid quantification of virus concentrations, thus demonstrating its full capabilities in the analysis of large macromolecular complexes.
Bacteriophages↗
Nanostructured sorbents for capture of cadmium species in combustion environments.
The pathways of cadmium species to form a submicrometer-sized aerosol in a combustion system exhaust were established. Cadmium oxide was the predominant species formed in the experiments and resulted in particles of a mean size of 26-63 nm with number concentrations in the range of 2-8 x 10(6) cm(-3). Two different nanostructured sorbents, a solid montmorillonite (MMT) and an in situ generated agglomerated silica, were used for capture of the cadmium species. The MMT sorbent was not stable at 1000 degrees C, and structural changes resulted. MMT did not suppress nucleation of cadmium species and partially captured it by weak physisorption as established by the leachability tests. In contrast, the in situ generated silica nanostructured agglomerates had a high surface area, suppressed nucleation of cadmium species vapors, and chemisorbed them effectively resulting in a firm binding, as compared to the MMT sorbent. There is an optimal temperature-time relationship at which the capture process is expected to be most effective. The leaching efficiency under these conditions was less than 3.2%. The nanostructured silica agglomerate size can be tuned for effective capture in existing particle control devices.
Air Pollutants↗
Hierarchical approach to model multilayer colloidal deposition in porous media.
Particle deposition is important in many environmental systems such as water and wastewater filtration, air pollution control, subsurface transport, biofilm formation and fouling, and thin film synthesis for use in remediation technologies. While continuum-level models have been developed to predict deposition dynamics in these systems, these models fail to explain transient dynamics of multilayer deposition from a mechanistic viewpoint. In this work, a multiscale approach has been developed to predict multiple layer irreversible colloidal deposition in the presence of interparticle electrostatic and van der Waals interactions in porous media. The approach combines the kinetic information obtained from the mesoscopic stochastic simulations of particle deposition with the macroscopic conservation equation describing colloidal transport. Sequential Brownian dynamics simulations are first performed by accounting for particle-particle (P-P) and particle-surface (P-S) interactions, and multilayered particle deposits are obtained. The available surface function quantifying the deposition kinetics is then obtained from the deposit microstructure. Deposition dynamics are studied at different ionic strengths and particle potentials that control the range and magnitude of interparticle interactions. Simulation results showed that the microstructure of the particle deposits formed under the influence of P-P and P-S electrostatic interactions exhibited significant variations with respect to ionic strength and could be qualitatively explained bythe interplay between the repulsive and attractive P-P and P-S interaction forces. The available surface function also varied significantly as a function of ionic strength. This basic understanding of the deposition dynamics at the mesoscale was then combined with the continuum-level transport equations to predict particle breakthrough curves in porous media. The approach is capable of capturing transient features of deposition dynamics, as demonstrated by the good agreement between the model predictions and the experimental observations.
Adsorption↗
Capture of water-borne colloids in granular beds using external electric fields: improving removal of Cryptosporidium parvum.
Suboptimal coagulation in water treatment plants often results in reduced removal efficiency of Cryptosporidium parvum oocysts by several orders of magnitude (J. AWWA 94(6) (2002) 97, J. AWWA 93(12) (2001) 64). The effect of external electric field on removal of C. parvum oocysts in packed granular beds was studied experimentally. A cylindrical configuration of electrodes, with granular media in the annular space was used. A negative DC potential was applied to the central electrode. No coagulants or flocculants were used and filtration was performed with and without application of an electric field to obtain improvement in removal efficiency. Results indicate that removal of C. parvum increased from 10% to 70% due to application of field in fine sand media and from 30% to 96% in MAGCHEM media. All other test particles (Kaolin and polystyrene latex microspheres) used in the study also exhibited increased removal in the presence of an electric field. Single collector efficiencies were also computed using approximate trajectory analysis, modified to account for the applied external electric field. The results of these calculations were used to qualitatively explain the trends in the experimental observations.
Animals↗
Nanoparticles and the environment.
Nanoparticles are a class of materials with properties distinctively different from their bulk and molecular counterparts. A critical review of the very broad topic of environmental nanoparticles is presented. Because of the vast nature of the topic, the review is focused primarily on gas-borne nanoparticles. The "life history of nanoparticles" is presented, tracking it from its formation to its potential use and eventual fate in the environment. Nanoparticle sources, anthropogenic emissions from industrial and occupational settings, and conversion and formation in the atmosphere are discussed. The ability to characterize and capture these nanoparticles (as would be necessary in a nanoparticle production system), as well as their control (of emissions from an industrial source) is discussed. A description on the use of nanoparticles in environmental technologies and the potential impact on the energy sector is provided. The potential effects on human health and the environment, both adverse and beneficial, are important aspects that need to be considered. As will be evident, the study of "environmental nanoparticles" is a new and fast-growing field. Much work remains to be done before we can fully harness the advantages of nanoparticles and ensure that there are no potential adverse consequences. A set of recommendations for additional work in each area is provided.
Environmental Monitoring↗
Nanoparticles and the environment.
Explore the source record for details and available documents.
Aerosols↗
A mechanistic model for mercury capture with in situ-generated titania particles: role of water vapor.
A mechanistic model to predict the capture of gas-phase mercury (Hg) species using in situ-generated titania nanosize particles activated by UV irradiation is developed. The model is an extension of a recently reported model for photochemical reactions by Almquist and Biswas that accounts for the rates of electron-hole pair generation, the adsorption of the compound to be oxidized, and the adsorption of water vapor. The role of water vapor in the removal efficiency of Hg was investigated to evaluate the rates of Hg oxidation at different water vapor concentrations. As the water vapor concentration is increased, more hydroxy radical species are generated on the surface of the titania particle, increasing the number of active sites for the photooxidation and capture of Hg. At very high water vapor concentrations, competitive adsorption is expected to be important and reduce the number of sites available for photooxidation of Hg. The predictions of the developed phenomenological model agreed well with the measured Hg oxidation rates in this study and with the data on oxidation of organic compounds reported in the literature.
Adsorption↗
A methodology to establish the morphology of ambient aerosols.
The morphology of ambient particulate matter (PM) is an important characteristic that seldom is measured and reported. A study was performed to determine the viability of a method to establish the distribution of shapes and the fractal dimensions of aggregates of ambient aerosols. Particles of PM with aerodynamic diameter less than or equal to 2.5 microm (PM2.5) were captured on different days via size-independent electrostatic precipitation at two sites in St. Louis and examined in a scanning electron microscope (SEM). Nonvolatile particles between 0.1 and 2.5 microm were readily identified via SEM. Particle shapes were classified as fibrous, spherical, agglomerated, or "other." A computer program using the nested-squares algorithm was developed and used to determine the fractal dimensions of the aggregates. More particles were collected at the St. Louis-Midwest Supersite on June 14, 2002, than were collected on the Washington University campus loading dock on May 31, 2002, but the campus samples had a higher percentage of aggregates. On one day of sampling at the Supersite, the aggregate fraction was highest in the morning (14.3% between 7:00 and 9:00 a.m.) and steadily declined during the day (1.3% between 5:00 and 7:00 p.m.). The fractal dimensions of the aerosols were 1.65 in the morning (7:00-9:00 a.m.), decreased to 1.49 (11:00 a.m.-1:00 p.m.), and then increased to 1.87 (5:00-7:00 p.m.). The results show that the fractal dimension is not a static value and that ambient aerosols are not perfectly spherical.
Aerosols↗
Multiscale simulation of irreversible deposition in presence of double layer interactions.
Sequential lattice Monte Carlo simulations, in which the transition probabilities are derived from the discrete form of the continuum-level mass conservation law, are used to predict the morphology of colloidal deposits. The simulations account for particle-surface (P-S) and particle-particle (P-P) electrostatic and van der Waals interactions. Simulation results for maximum coverage for monolayer deposition are in quantitative agreement with the hard-sphere RSA jamming limit. Moreover, as reported in earlier studies, monolayer simulations in the absence of P-S interactions qualitatively predict the monotonic increases in fractional coverage with increasing ionic strength, characterized by the Debye screening length (kappa a). Monolayer simulations with P-S interactions show that the dependence of fractional coverage on kappa a is strongly influenced by the ratio of particle to surface potentials (Psi(p)/Psi(s)). P-S and P-P forces achieve their respective maximum at different values of kappa a leading to a nonmonotonic trend in surface coverage as a function of kappa a. These results indicate that the incorporation of P-S interactions into colloidal deposition studies allows more accurate interpretation of the experimental data. In multilayer deposition simulations, balance between long-ranged weak interactions and short-ranged strong interactions between P-P and P-S, coupled with physical screening effects, resulted in widely varying coverages with height of the deposit, ionic strength, and Psi(p)/Psi(s). Moreover, fractal dimension of the deposit ranged from approximately 1 (kappa a << 1) to 1.7 (kappa a >> 1). Qualitative kinetic analysis showed widely varying deposition rates in different layers depending on Psi(p)/Psi(s) and ionic strength. The multilayer system approached the monolayer system in the limit kappa a--> infinity and Psi(p)/Psi(s)--> infinity.
Journal Article↗
Concentration gradient patterns of aerosol particles near interstate highways in the Greater Cincinnati airshed.
The objective of this study was to determine if there is an exposure gradient in particulate matter concentrations for people living near interstate highways, and to determine how far from the highway the gradient extends. Air samples were collected in a residential area of Greater Cincinnati in the vicinity of two major highways. The measurements were conducted at different distances from the highways by using ultrafine particle counters (measurement range: 0.02-1 microm), optical particle counters (0.3-20 microm), and PM2.5 Harvard Impactors (0.02-2.5 microm). The collected PM2.5 samples were analyzed for mass concentration, for elemental and organic carbon, and for elemental concentrations. The results show that the aerosol concentration gradient was most clearly seen in the particle number concentration measured by the ultrafine particle counters. The concentration of ultrafine particles decreased to half between the sampling points located at 50 m and 150 m downwind from the highway. Additionally, elemental analysis revealed a gradient in sulfur concentrations up to 400 m from the highway in a residential area that does not have major nearby industrial sources. This gradient was qualitatively attributed to the sulfate particle emissions from diesel engine exhausts, and was supported by the concentration data on several key elements indicative of traffic sources (road dust and diesel exhaust). As different particulate components gave different profiles of the diesel exposure gradient, these results indicate that no single element or component of diesel exhaust can be used as a surrogate for diesel exposure, but more comprehensive signature analysis is needed. This characterization is crucial especially when the exposure data are to be used in epidemiological studies.
Air Pollutants↗
Separation and capture of CO2 from large stationary sources and sequestration in geological formations.
Explore the source record for details and available documents.
Carbon Dioxide↗
Development and demonstration of an explicit lumped-parameter biofilter model and design equation incorporating monod kinetics.
Biofiltration is an economical air pollution control (APC) technology, particularly suitable for the treatment of air-streams having high flow rates and low concentrations of volatile organic compounds (VOCs). This technology utilizes enzymatic catalysis at ambient conditions to mineralize such pollutants to CO2, H2O, and salts. A pilot-scale study conducted for more than 4 years investigated the development of a new biofiltration technology employing trickle bed air biofilters (TBABs). Following the completion of this experimental study, additional data analysis was performed to develop a simple lumped-parameter biofilter model, assuming first-order kinetics. This model related the observed biofilter performance to the principle independent physical, thermodynamic, and biochemical parameters. The initial model has subsequently been expanded to incorporate Monod kinetics. In this paper, the development and use of the final explicit lumped-parameter biofilter model and design equation, incorporating Monod kinetics, are presented. To facilitate the application of this model, practical procedures are also presented for the determination of VOC solubility, VOC biokinetic Monod parameters, and the maximum practical biofilter inlet VOC concentration.
Air Pollutants↗
Hg reactions in the presence of chlorine species: homogeneous gas phase and heterogeneous gas-solid phase.
The kinetics of Hg chlorination (with HCl) was studied using a flow reactor system with an online Hg analyzer, and speciation sampling using a set of impingers. Kinetic parameters, such as reaction order (alpha), overall rate constant (k'), and activation energy (Ea), were estimated based on the simple overall reaction pathway. The reaction order with respect to C(Hg), k', and Ea were found to be 1.55, 5.07 x 10(-2) exp(-1939.68/T) [(microg/m3)(-055)(s)(-1)]. and 16.13 [kJ/ mol], respectively. The effect of chlorine species (HCl, CH2Cl2) on the in situ Hg capture method previously developed (28) was also investigated. The efficiency of capture of Hg by this in situ method was higher than 98% in the presence of chlorine species. Furthermore, under certain conditions, the presence of chlorine enhanced the removal of elemental Hg by additional gas-phase oxidation.
Environmental Pollutants↗