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      Human occupant contribution to secondary aerosol mass in the indoor environment

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          Abstract

          Occupancy in indoor spaces can contribute to indoor aerosol mass via reactions of oxidants such as ozone with skin constituents and subsequent partitioning of those oxidation product to existing aerosol.

          Abstract

          Humans impact indoor air quality directly via emissions from skin, breath, or personal care products, and indirectly via reactions of oxidants with skin constituents, or with skin that has been shed. However, separating the influence of the many emissions and their oxidation products from the influence of outdoor-originated aerosols has been a challenge. Indoor and outdoor aerosols were alternatively sampled at 4 minute time resolution with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in a classroom with student occupants at regular intervals per university class schedule. Mass spectral analysis showed aerosol enhancements of oxidized and unoxidized hydrocarbon ion families during occupied periods, especially at ion fragments larger than m/ z 100 and double bond equivalents consistent with squalene (C 30H 50) and its oxidized products from reaction with ozone, indicative of the secondary nature of the aerosol mass. Individual hydrocarbon mass fragments consistent with squalene fragmentation, including C 5H 9 +, and C 6H 9 + were especially enhanced with room occupancy. Emissions of individual organic fragment ions were estimated using a model accounting for outdoor aerosols and air exchange. This showed occupancy related emissions at smaller fragments (C 3H 5 +, C 4H 9 +) that despite reflecting mostly outdoor-originated aerosols transported indoors, also show enhancements from occupant emissions indoors. Total emission of all fragments was 17.6 μg β −1 h −1 above unoccupied levels, translating to approximately 25% increase in organic aerosol mass concentration in the classroom during an occupied hour with a median occupied ozone loss ( β). Human occupants, therefore, represent an additional mass burden of organic aerosol, especially in poorly ventilated or highly occupied indoor spaces.

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          Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer.

          The application of mass spectrometric techniques to the real-time measurement and characterization of aerosols represents a significant advance in the field of atmospheric science. This review focuses on the aerosol mass spectrometer (AMS), an instrument designed and developed at Aerodyne Research, Inc. (ARI) that is the most widely used thermal vaporization AMS. The AMS uses aerodynamic lens inlet technology together with thermal vaporization and electron-impact mass spectrometry to measure the real-time non-refractory (NR) chemical speciation and mass loading as a function of particle size of fine aerosol particles with aerodynamic diameters between approximately 50 and 1,000 nm. The original AMS utilizes a quadrupole mass spectrometer (Q) with electron impact (EI) ionization and produces ensemble average data of particle properties. Later versions employ time-of-flight (ToF) mass spectrometers and can produce full mass spectral data for single particles. This manuscript presents a detailed discussion of the strengths and limitations of the AMS measurement approach and reviews how the measurements are used to characterize particle properties. Results from selected laboratory experiments and field measurement campaigns are also presented to highlight the different applications of this instrument. Recent instrumental developments, such as the incorporation of softer ionization techniques (vacuum ultraviolet (VUV) photo-ionization, Li+ ion, and electron attachment) and high-resolution ToF mass spectrometers, that yield more detailed information about the organic aerosol component are also described. (c) 2007 Wiley Periodicals, Inc.
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            A review of the volatiles from the healthy human body.

            A compendium of all the volatile organic compounds (VOCs) emanating from the human body (the volatolome) is for the first time reported. 1840 VOCs have been assigned from breath (872), saliva (359), blood (154), milk (256), skin secretions (532) urine (279), and faeces (381) in apparently healthy individuals. Compounds were assigned CAS registry numbers and named according to a common convention where possible. The compounds have been grouped into tables according to their chemical class or functionality to permit easy comparison. Some clear differences are observed, for instance, a lack of esters in urine with a high number in faeces. Careful use of the database is needed. The numbers may not be a true reflection of the actual VOCs present from each bodily excretion. The lack of a compound could be due to the techniques used or reflect the intensity of effort e.g. there are few publications on VOCs from blood compared to a large number on VOCs in breath. The large number of volatiles reported from skin is partly due to the methodologies used, e.g. collecting excretions on glass beads and then heating to desorb VOCs. All compounds have been included as reported (unless there was a clear discrepancy between name and chemical structure), but there may be some mistaken assignations arising from the original publications, particularly for isomers. It is the authors' intention that this database will not only be a useful database of VOCs listed in the literature, but will stimulate further study of VOCs from healthy individuals. Establishing a list of volatiles emanating from healthy individuals and increased understanding of VOC metabolic pathways is an important step for differentiating between diseases using VOCs.
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              Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications

              Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), and organic mass-to-organic carbon (OM : OC) ratios, and of carbon oxidation state ( OS C ) for a vastly expanded laboratory data set of multifunctional oxidized OA standards. For the expanded standard data set, the method introduced by Aiken et al. (2008), which uses experimentally measured ion intensities at all ions to determine elemental ratios (referred to here as "Aiken-Explicit"), reproduces known O : C and H : C ratio values within 20% (average absolute value of relative errors) and 12%, respectively. The more commonly used method, which uses empirically estimated H 2 O + and CO + ion intensities to avoid gas phase air interferences at these ions (referred to here as "Aiken-Ambient"), reproduces O : C and H : C of multifunctional oxidized species within 28 and 14% of known values. The values from the latter method are systematically biased low, however, with larger biases observed for alcohols and simple diacids. A detailed examination of the H 2 O + , CO + , and CO 2 + fragments in the high-resolution mass spectra of the standard compounds indicates that the Aiken-Ambient method underestimates the CO + and especially H 2 O + produced from many oxidized species. Combined AMS–vacuum ultraviolet (VUV) ionization measurements indicate that these ions are produced by dehydration and decarboxylation on the AMS vaporizer (usually operated at 600 °C). Thermal decomposition is observed to be efficient at vaporizer temperatures down to 200 °C. These results are used together to develop an "Improved-Ambient" elemental analysis method for AMS spectra measured in air. The Improved-Ambient method uses specific ion fragments as markers to correct for molecular functionality-dependent systematic biases and reproduces known O : C (H : C) ratios of individual oxidized standards within 28% (13%) of the known molecular values. The error in Improved-Ambient O : C (H : C) values is smaller for theoretical standard mixtures of the oxidized organic standards, which are more representative of the complex mix of species present in ambient OA. For ambient OA, the Improved-Ambient method produces O : C (H : C) values that are 27% (11%) larger than previously published Aiken-Ambient values; a corresponding increase of 9% is observed for OM : OC values. These results imply that ambient OA has a higher relative oxygen content than previously estimated. The OS C values calculated for ambient OA by the two methods agree well, however (average relative difference of 0.06 OS C units). This indicates that OS C is a more robust metric of oxidation than O : C, likely since OS C is not affected by hydration or dehydration, either in the atmosphere or during analysis.
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                Author and article information

                Journal
                ESPICZ
                Environmental Science: Processes & Impacts
                Environ. Sci.: Processes Impacts
                Royal Society of Chemistry (RSC)
                2050-7887
                2050-7895
                August 14 2019
                2019
                : 21
                : 8
                : 1301-1312
                Affiliations
                [1 ]Department of Civil, Architectural, and Environmental Engineering
                [2 ]Drexel University
                [3 ]Philadelphia
                [4 ]USA
                [5 ]Department of Chemistry
                Article
                10.1039/C9EM00097F
                b92dc9d6-4d99-4e7d-b2dd-2a325bc94a8d
                © 2019

                Free to read

                http://rsc.li/journals-terms-of-use#chorus

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