skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Digital Microfluidics for the Detection of Selected Inorganic Ions in Aerosols
A prototype aerosol detection system is presented that is designed to accurately and quickly measure the concentration of selected inorganic ions in the atmosphere. The aerosol detection system combines digital microfluidics technology, aerosol impaction and chemical detection integrated on the same chip. Target compounds are the major inorganic aerosol constituents: sulfate, nitrate and ammonium. The digital microfluidic system consists of top and bottom plates that sandwich a fluid layer. Nozzles for an inertial impactor are built into the top plate according to known, scaling principles. The deposited air particles are densely concentrated in well-defined deposits on the bottom plate containing droplet actuation electrodes of the chip in fixed areas. The aerosol collection efficiency for particles larger than 100 nm in diameter was higher than 95%. After a collection phase, deposits are dissolved into a scanning droplet. Due to a sub-microliter droplet size, the obtained extract is highly concentrated. Droplets then pass through an air/oil interface on chip for colorimetric analysis by spectrophotometry using optical fibers placed between the two plates of the chip. To create a standard curve for each analyte, six different concentrations of liquid standards were chosen for each assay and dispensed from on-chip reservoirs. The droplet mixing was completed in a few seconds and the final droplet was transported to the detection position as soon as the mixing was finished. Limits of detection (LOD) in the final droplet were determined to be 11 ppm for sulfate and 0.26 ppm for ammonium. For nitrate, it was impossible to get stable measurements. The LOD of the on-chip measurements for sulfate was close to that obtained by an off-chip method using a Tecan spectrometer. LOD of the on-chip method for ammonium was about five times larger than what was obtained with the off-chip method. For the current impactor collection air flow (1 L/min) and 1 h collection time, the converted LODs in air were: 0.275 μg/m3 for sulfate, 6.5 ng/m3 for ammonium, sufficient for most ambient air monitoring applications.  more » « less
Award ID(s):
1408241
PAR ID:
10156895
Author(s) / Creator(s):
; ; ;
Date Published:
Journal Name:
Sensors
Volume:
20
Issue:
5
ISSN:
1424-8220
Page Range / eLocation ID:
1281
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Organic compounds in the atmosphere play a pivotal role in atmospheric chemistry, and clouds are significant in the genesis and alteration of these compounds. Di-carboxylic organic anions such as oxalate serve as tracers for aqueous processing. This poster details our findings from summer measurements of three major organic acids (formic acid, acetic acid, oxalic acid), as well as inorganic anions (sulfate, chloride, nitrate) and cations (sodium, potassium, ammonium, calcium, magnesium) in cloud water, aerosol, and cloud droplet residual samples collected at the summit of Whiteface Mountain (WFM) in the Adirondack Mountains, northern New York State. We also evaluate the contribution of these organic acids to water-soluble organic carbon (WSOC) concentrations. Previous studies have explored the oxalate: WSOC ratio with ozone levels, aiming to deduce the influence of biogenic Volatile Organic Compounds (VOCs) on Secondary Organic Aerosol (SOA) formation from nearby forest ecosystems. Our poster presents new observations that significantly broaden this understanding by comparing to diverse global environments and analyzing both cloud water and aerosol phases. Additionally, we introduce oxalate: sulfate ratios from our dataset, proposed by other researchers as a key indicator of aqueous processing due to the enhanced production rates of these ions by liquid water content (sulfate ion) or droplet surface area (oxalate ion). We compare the observed range of oxalate: sulfate ratios with those from field campaigns conducted in other regions. Moreover, for the first time, we examine the relationship between ammonium and organic acids across cloud water, aerosol, and droplet residual samples collected in 2023, and discuss the influence of wildfire smoke on these dynamics. 
    more » « less
  2. Nicole Riemer (Ed.)
    Aerosol particles in the atmosphere have the ability to uptake water and form droplets. The droplets formed can interact with solar radiation (indirect effect of aerosols) and influence the net radiative forcing. However, the magnitude of change in radiative forcing due to the indirect effect of aerosols remains uncertain due to the high variance in aerosol composition and mixing states, both spatial and temporally. As such, there is a need to measure the water-uptake of different aerosol particle groups under controlled conditions to gain insight into the water-uptake of complex ambient systems. In this work, the water-uptake (hygroscopicity) of internally and externally mixed ammonium sulfate – organic binary mixtures were directly measured via three methods and compared to droplet growth prediction models. We found that subsaturated water-uptake of ammonium sulfate-organic mixtures agreed with their supersaturated hygroscopicity, and mixing state information was able to be retrieved at both humidity regimes. In addition, we found that solubility-adjusted models may not be able to capture the water-uptake of viscous particles, and for soluble organic aerosol particles, bulk solubility may not be comparable to their solubility in a droplet. This work highlights the importance of using multiple complementary water-uptake measurement instruments to get a clearer picture of mixed aerosol particle hygroscopicity, especially for increasingly complex systems. 
    more » « less
  3. Ambient aerosol particles can undergo dynamic mixing processes as they coagulate with particles from other air masses and emission sources. Therefore, aerosols exist in a spectrum, from externally mixed to internally mixed. The mixing state of aerosols can affect their ability to uptake water (hygroscopicity) and their cloud condensation nuclei (CCN) activity, modifying their contribution to the planet’s total radiative budget. However, current water-uptake measurement methods may not be able to capture the complex mixing state. In this research, the dynamic mixing process was simulated by the particle-resolved aerosol model PartMC and also created by experiments in a laminar flow mixing tube. The mixing evolution of ammonium sulfate and sucrose binary mixtures were observed along with the changes in their water uptake properties expressed as the single hygroscopicity parameter, κ. The use of a mixing simulation in conjunction with experiments allow for better identification of the particle mixing state and the particle water uptake and show that no one kappa value can capture the complexity of mixing across the mixed particle size distribution. In other words, the PartMC simulations can be used as a guiding tool to interpret a system’s mixing state based on its experimental droplet activation spectra. This work demonstrates the importance of the integration and use of mixing models to aid in mixing state determination and hygroscopicity measurements of mixed systems. 
    more » « less
  4. Abstract The Asian Summer Monsoon (ASM) convection transports aerosols and their precursors from the boundary layer to the upper troposphere and lower stratosphere (UTLS). This process forms an annually recurring aerosol layer near the tropopause. Recent observations have revealed a distinct property of the aerosol layer over the ASM region, it is nitrate‐rich. We present a newly implemented aerosol formation algorithm that enhances the representation of nitrate aerosol in the Community Aerosol and Radiation Model for Atmospheres (CARMA) coupled with the Community Earth System Model (CESM). The simulated aerosol chemical composition, as well as vertical distributions of aerosol size and mass, are evaluated using in situ and remote sensing observations. The simulated concentrations (ammonium, nitrate, and sulfate) and size distributions are generally within the error bars of data. We find nitrate, organics, and sulfate contribute significantly to the UTLS aerosol concentration between 15°–45°N and 0°–160°E. The two key formation mechanisms of nitrate‐containing aerosols in the ATAL are ammonium neutralization to form ammonium nitrate in regions where convection is active, and condensation of nitric acid in regions of cold temperature. Furthermore, including nitrate formation in the model doubles the surface area density in the tropical tropopause region between 15°–45°N and 0°–160°E, which alters the chlorine partitioning and subsequently impacts the rate of ozone depletion. 
    more » « less
  5. Isoprene has a strong effect on the oxidative capacity of the troposphere due to its abundance. Under low-NOx conditions, isoprene oxidizes to form isoprene-derived epoxydiols (IEPOX), contributing significantly to secondary organic aerosol (SOA) through heterogeneous reactions. In particular, organosulfates (OSs) can form from acid-driven reactive uptake of IEPOX onto preexisting particles followed by nucleophilic addition of inorganic sulfate, and they are an important component of SOA mass, primarily in submicron particles with long atmospheric lifetimes. Fundamental understanding of SOA and OS evolution in particles, including the formation of new compounds by oxidation as well as corresponding viscosity changes, is limited, particularly across relative humidity (RH) conditions above and below the deliquescence of typical sulfate aerosol particles. In a 2-m3 indoor chamber held at various RH values (30 – 80%), SOA was generated from reactive uptake of gas-phase IEPOX onto acidic ammonium sulfate aerosols (pH = 0.5 – 2.5) and then aged in an oxidation flow reactor (OFR) for 0 – 24 days of equivalent atmospheric ·OH exposure. We investigated the extent of inorganic sulfate conversion to organosulfate, formation of oligomers, single-particle physicochemical properties, such as viscosity and phase state, and oxidation kinetics. Chemical composition of particle-phase species, as well as aerosol morphological changes, are analyzed as a function of RH, oxidant exposure times, and particle acidity to better understand SOA and OS formation and destruction mechanisms in the ambient atmosphere. 
    more » « less