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Development and Applications of Opposed Migration Aerosol Classifiers (OMACs)

Citation

Mui, Wilton (2017) Development and Applications of Opposed Migration Aerosol Classifiers (OMACs). Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/Z9T72FF1. http://resolver.caltech.edu/CaltechTHESIS:09062016-204048228

Abstract

Particle electrical mobility classification has made important contributions in atmospheric and climate science, public health and welfare policy, and nanotechnology. The measurement of the particle size distribution is integral to characterization of the sub-micrometer aerosol particle population. The differential mobility analyzer (DMA) has been the primary instrument for such measurements. Aerosol particles are transmitted through the DMA on the condition that their migration time across an electrode separation distance is approximately equal to the advective transport time from the inlet to the outlet; these two travel times are induced by an electric field between the electrodes and an orthogonal particle-free carrier gas flow. However, scientific interest has increasingly shifted toward both the nanometer-scale particle size distribution and the miniaturization of instruments. The classical DMA suffers from severe resolution degradation and diffusional losses of nanometer-scale particles, as well as being ill-suited for lightweight, low-power applications. It is relatively recently that miniaturization of DMAs for portable applications has appeared in the scientific literature. Additionally, an abundance of efforts on DMA design have yielded instruments that can probe the nanometer-scale particle size regime, though their use is restricted to the laboratory as they require powerful pumps and operate at near-turbulent flow conditions.

The opposed migration aerosol classifier (OMAC) is a novel concept for particle electrical mobility classification introduced about a decade ago. In contrast to the DMA, the OMAC transmits particles on the condition that their migration velocity in an electric field is approximately equal to the advective transport velocity by a particle-free flow; the migration velocity is induced by an electric field between two porous electrodes, through which a particle-free cross-flow moves in an anti-parallel direction to the electric field. Because of this flow field arrangement, the length scale over which diffusion must act to affect resolution is the entire electrode separation distance in the OMAC, whereas in the DMA it is smaller by about a factor of the sample-to-carrier gas flow rate ratio. As a result, resolution degradation due to diffusion occurs at a lower operating voltage in the OMAC compared to the DMA. Not only does this suggest a larger dynamic range for the OMAC, but also the capability to classify nanometer-scale particles with greater resolution and lower operating voltages and flow rates.

Motivated by the theoretical advantages of an OMAC compared to a DMA, this thesis details the design and characterization of OMAC classifiers to verify the performance of realized OMACs. The capabilities of prototype radial geometry OMACs were first investigated. They demonstrated sub-20 nm particle diameter classification at high resolution using modest flow rates, making them amenable to non-laboratory applications. Additionally, the delayed resolution degradation of OMACs was validated by the maintenance of resolution at operating voltages below those at which a DMA would have experienced severely degraded resolution.

Various applications were then carried out to validate the use of OMACs in both nanometer-scale and sub-micrometer particle size regimes. The first OMAC application was in the field of biomolecule analysis, in which the radial OMAC was operated as an ion mobility spectrometer coupled to a mass spectrometer to resolve conformations of sub-2 nm biomolecules. The resolving power of the radial OMAC was high enough to differentiate peptide stereoisomers and populations of thermally-induced biomolecule conformations.

In the aerosol measurement field, aerosol particle size distributions are typically obtained by passing the sample through an ionization source to impart charges on the sample particles, before mobility separation and detection. The detected signal must be inverted, using detector efficiencies, classifier transfer functions, and charge distributions, to obtain the true particle size distribution. While detector efficiencies and classifier transfer functions are typically well-quantified for the specific instruments used in the measurement, the charge distribution is almost never calculated for the specific measurement conditions. This is due both to the computational expense of, as well as the present impracticability of obtaining all the information needed for carrying out such calculations. Aerosol scientists typically use one parameterization of the charge distribution, regardless of the measurement conditions. Thus, the charge distribution represents the greatest source of bias in particle size distribution measurements. Having demonstrated high resolution of sub-2 nm ions, the radial OMAC was then used to obtain mobility distributions of gas ions formed in a bipolar aerosol charger. These ion mobility distributions were then used to quantify the particle size distribution bias due to the use of the common charge distribution parameterization.

In atmospheric nucleation field, the radial OMAC was deployed as part of an airborne particle detection payload over a large cattle feedlot. Again, the radial OMAC demonstrated the ability to obtain nanometer-scale particle size distributions, that, when paired with a concurrently-deployed DMA, allowed for the measurement of ambient particle size distributions over the entire sub-micrometer size range. A spatially-dense set of such particle size distributions allowed for the calculation of particle growth rates from a clear nucleation event from cattle feedlot emissions.

Finally, OMACs were evaluated for their performance at low-flow rate operation to obtain sub-micron particle size distribution for deployment as portable exposure monitors, distributed network area monitors, and unmanned aerial vehicle instrumentation. The radial OMAC showed high fidelity to a reference instrument in reported ambient particle size distributions for nearly 48 hours of unattended operation. A planar geometry OMAC prototype was designed and characterized as well, indicating design and construction issues that caused deviations from ideal behavior. The planer OMAC qualitatively agreed with a reference instrument in reported ambient particle size distributions for about 12 hours of unattended operation. Both radial and planar OMACs were more compact, lower in weight, and less demanding in power consumption than a classical DMA, showing high potential for further miniaturized instrumentation development.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:differential mobility analysis, aerosol measurement, particle size distribution, opposed migration aerosol classifier
Degree Grantor:California Institute of Technology
Division:Engineering and Applied Science
Major Option:Environmental Science and Engineering
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Flagan, Richard C. (advisor)
  • Seinfeld, John H. (co-advisor)
Thesis Committee:
  • Flagan, Richard C. (chair)
  • Seinfeld, John H.
  • Beauchamp, Jesse L.
  • Okumura, Mitchio
Defense Date:4 January 2017
Non-Caltech Author Email:wiltonmui88 (AT) gmail.com
Record Number:CaltechTHESIS:09062016-204048228
Persistent URL:http://resolver.caltech.edu/CaltechTHESIS:09062016-204048228
DOI:10.7907/Z9T72FF1
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-15-5027-2015DOIArticle reproduced in Appendix J.
https://doi.org/10.1021/ac400580uDOIArticle adapted for Chapter 3.
https://doi.org/10.1073/pnas.1300262110DOIArticle reproduced in Appendix I.
https://doi.org/10.1021/es301138yDOIArticle reproduced in Appendix H.
ORCID:
AuthorORCID
Mui, Wilton0000-0003-3065-1296
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:9917
Collection:CaltechTHESIS
Deposited By: Wilton Mui
Deposited On:13 Feb 2017 20:12
Last Modified:13 Feb 2017 20:12

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