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A single usage of a kitchen degreaser can alter indoor aerosol composition for days Jaroslav Schwarz, Otakar Makeš, Jakub Ondrá#ek, Michael Cusack, Nicholas Talbot, Petr Vodi#ka, Lucie Kubelova, and Vladimir Zdimal Environ. Sci. Technol., Just Accepted Manuscript • Publication Date (Web): 27 Apr 2017 Downloaded from http://pubs.acs.org on April 27, 2017

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Environmental Science & Technology

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A single usage of a kitchen degreaser can alter indoor

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aerosol composition for days

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Jaroslav Schwarz*, Otakar Makeš, Jakub Ondráček, Michael Cusack, Nicholas Talbot, Petr

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Vodička, Lucie Kubelová, Vladimír Ždímal

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Institute of Chemical Process Fundamentals of the CAS, Prague, Czech Republic

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Abstract

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To the best of our knowledge, this study represents the first observation of multi-day persistence

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of an indoor aerosol transformation linked to a kitchen degreaser containing mono-ethanol amine

10

(MEA). MEA remaining on the cleaned surfaces and on a wiping paper towel in a trash can was

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able to transform ammonium sulfate and ammonium nitrate into (MEA)2SO4 and (MEA)NO3. This

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influence persisted for at least 60 hours despite a high average ventilation rate. The influence was

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observed using both offline (filters, impactors, and ion chromatography analysis) and online

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(compact time-of-flight aerosol mass spectrometer) techniques. Substitution of ammonia in

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ammonium salts was observed not only in aerosol but also in particles deposited on a filter before

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the release of MEA. The similar influence of other amines is expected based on literature data.

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This influence represents a new pathway for MEA exposure of people in an indoor environment.

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The stabilizing effect on indoor nitrate also causes higher indoor exposure to fine nitrates.

ACS Paragon Plus Environment

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TOC art

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Introduction

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Indoor aerosol studies are important because people spend approximately 80% of their lives

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indoors, and aerosols can have negative health effects, as observed in many studies1. Indoor

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aerosols can originate as outdoor aerosol transported through windows and wall leaks2. In the

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absence of indoor aerosol sources, the levels of indoor aerosol are always lower than outdoor

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aerosol levels, and the difference depends on the natural air exchange rate in the absence of

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filtration devices. The size dependence of the indoor/outdoor ratio resulting from different particle

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removal processes is well known.

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However, when indoor sources, such as smoking, cooking, open fire heating or cleaning, are

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present, these sources can easily dominate indoor aerosol concentrations and affect the overall

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aerosol chemical composition. Even humans act as aerosol source that adds particles to the overall

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indoor aerosol content.

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The chemical transformation of particles transported from outside to the indoor environment is

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well known and frequently observed for the case of ammonium nitrates3–5. However, little is

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known about transformations of indoor aerosols under the influence of the broad collection of

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chemicals we use to keep our homes clean and at the desired level of sterility.


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One family of substances often found in the domestic environment is aminium salts, which are

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used in different surface active detergents. By examining manufacturer data and chemically

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analyzing this cleaner, we found that not only aminium salts are used in the water solution of

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degreasing solutes but also free amines such as mono-ethanol amine (MEA).

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The role of amines and aminium salts in ambient atmospheric aerosols has been recognized

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relatively recently6, leading to a growing number of papers dealing with this subject. The influence

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of amines on ambient atmospheric nucleation has been studied both theoretically7 and

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experimentally8,9. Amines have been found in the ultrafine fraction of ambient aerosol, and there

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are only a few papers dealing with their possible effects. Recently, aminium salts were suggested

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to be at least partially responsible for new particle formation events10, and their ability to thermally

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stabilize nitrates was studied by Salo et al. (2011)11. The growing interest in aminium salts in

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atmospheric aerosol has also led to studies of their relevant properties12–14 and their chemical

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reactions with atmospherically relevant compounds9,15–19. Very recently Chu and Chan (2017)20

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studied uptake of dimethyl amine by ammonium sulphates and its mixture with sucrose. The

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toxicology of amines was reviewed by Knaak et al. (1997)21; more recently, the toxicology of

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MEA was studied by Kamijo et al. (2007)22.

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Two papers have also described the influence of sulfuric acid emissions on MEA aerosol during

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the CO2 capture process23,24, suggesting the formation of MEA sulfate in the aerosol phase.

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In this study, and we believe for the first time in the context of a common indoor environment, we

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describe the ability of mono-ethanol amine, a constituent of a commercial degreaser solution for

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cleaning kitchens, to replace ammonium in inorganic salts in the indoor environment. In this case,

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ammonium is replaced mainly in its sulfate and nitrate salts in the inorganic aerosol that usually

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forms up to half of PM2.5 aerosol mass in indoor environments. Both complete and partial


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replacement was recorded in our experiment, depending on the mode of degreaser usage and the

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indoor activities that followed. Moreover, the dynamics of the pollution are described using a

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combination of different aerosol instrumentation and analytical techniques during a

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comprehensive indoor/outdoor experiment using both offline and online sampling techniques in

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an experimental room at an Institute of Chemical Process Fundamentals (ICPF) facility. This

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configuration is similar to one used in our previous paper4, but here, the investigation was

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substantially enriched using a in house built humidity tandem differential mobility analyzer

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(HTDMA)25, field OC/EC analyzer (Sunset Laboratory Inc., Tigard, USA), and compact time-

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of-flight aerosol mass spectrometer (C-ToF-AMS, referred further as AMS, Aerodyne Research,

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Inc., Billerica, USA)26. A complete overview of the campaign and its results are provided

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elsewhere26. In this paper, the newly recognized effects of cleaning chemicals used indoors are

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described with focus on change in indoor aerosol chemical composition.

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Experimental procedures

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The offline sampling used PM1 and PM10 sampling heads with Leckel pumps (Sven Leckel

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GmbH, Berlin, Germany) and SDI and BLPI cascade impactors to collect aerosol samples in both

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indoor and outdoor environments in parallel. Samples were collected for 23 h. The filter holders

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were loaded with pre-combusted (800°C, 3 h) quartz fiber filters (Pall Tissuquartz, 47 mm). For

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PM1, two filters in series were used to mitigate the possible adsorption artifacts for the OC/EC

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analyses. The filters and BLPI samples were analyzed using gravimetry and ion chromatography.

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More details about the sampling campaign can be found in Talbot et al. (2016)27. Here, the

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description concentrates only on the experimental details relevant to this paper.


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In addition to other sources, the influence of a W5 degreaser (Lidl Stiftung & Co. KG, Neckarsulm,

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Germany) sprayed on kitchen furniture surfaces was studied. Similar degreasers are sold under

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different names globally. The spray composition, as declared by the producer, is as follows

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(without concentrations): water, sodium C13-17 alkane sulfonate, mono-ethanolamine, MEA-

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palm kernelate, trisodium n,n-bis (carboxymethyl)-ß-alanine, perfume, limonene. The IC

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chromatography analysis showed more than 5% (w/w) of MEA in the solution.

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The following experiment was completed twice. During the first cleaner usage on September 1,

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2014, the cleaner was applied at 6:30 p.m. for 1 min. At that time, 24 h filter sampling of PM1 and

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PM10 aerosol was already underway, beginning at 10 a.m. The AMS, SMPS, APS, and HTDMA

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were also continuously running during that whole period. The next day (September 2, 2014),

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between 9 a.m. and 10 a.m., the filters were changed, and the BLPI and SDI were turned on at the

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same time. The micro-ventilation and ventilator above the electrical stove were also turned on. No

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additional indoor source was used over the next 24 h, but the micro-ventilation and ventilator were

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switched off at 15:59 because a coal-burning smell was detected at the site. On the third day

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(09/03/2014) at 9:44 a.m., the surface was wiped, and new filters were loaded. At 16:00, an outdoor

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barbecue was used to visualize the entrainment of aerosols to the indoor space. No impactors were

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running during that time. On September 4th and 5th, other indoor sources were tested. On September

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6th, the same cleaning solution was used at 9:50 a.m., and the doors were closed at 10 a.m. Only

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the online instruments, including the AMS, were running at that point and continued to run until

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the end of campaign, on September 8th at 11:08.

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The quartz fiber filter samples and the BLPI impactor foils were weighted and stored in a freezer

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until the analysis of water soluble ions was completed using a Dionex 5000 system that enables

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parallel analysis of both anions and cations. Two different calibrations were used for cations; one


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of them included six amine standards in addition to the standard cations (Na+, NH4+, K+, Mg2+,

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Ca2+). All amines (mono-ethanolamine (MEA), tri-ethanolamine (TEA), tri-ethylamine (TA), tri-

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methylamine (TMA), methoxypropylamine (MPA), and tetra-methylammonium (TMAH)) used

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in calibration were separated from other cations; however, complete separation of ammonium and

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MEA was not achieved (Fig. 1).

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Figure 1. IC separation of basic cations and six amines.

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AMS determination of MEA aerosol concentrations

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The AMS data were first evaluated using standard procedures described in Allan et al. (2004)28

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and for our instrument in Kubelová et al. (2015)29. Although c-ToF-AMS is not normally used for

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the determination of individual substance concentrations, with the exception of certain inorganic

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species, we have found a semi-quantitative way to determine MEA concentrations in the aerosol

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phase during part of the sampling period. The determination was based on the difference in ratio

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of m/zNO3 30 and m/zNO3 46, for normal ambient conditions (the ratio is normally relatively stable

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in ambient aerosol for a given AMS instrument) and the same ratio for period under the MEA

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influence. The concentration of MEA in aerosol was determined from balance of masses m/zNO3

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30 and m/zNO3 46 originally attributed to nitrates and their ambient ratio and the ratio of same

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masses found during calibration using MEA sulfate aerosol. The details of this procedure are


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similar to those reported by Murphy et al. (2007)30, who characterized aminium nitrate salts

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(including MEA nitrate) in a chamber study using c-ToF AMS and noted the influence of amines

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on m/z 30, and are given in Supplement 1. The ratio is influenced by the presence of other sources

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(particularly combustion); thus, only data without the strong influence of another source are

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presented. Comparison of mass spectra measured for MEA sulfate showed a substantial effect on

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mass m/z 30 that is normally attributed to nitrates (Fig. S2). No species dependent collection

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efficiency (CE) was applied here.

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Results and discussion

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Average ratios of PM1, PM10, and compounds with no indoor sources in the indoor and outdoor

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environments

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Several sampling days throughout the campaign were devoted to determining the indoor/outdoor

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relationship of aerosol without the influence of any major indoor source. Various ventilation

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scenarios were used during these sampling days to test the influence of ventilation rate on indoor

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concentrations. Table 1 contains the results of the average indoor-to-outdoor ratios of the main

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aerosol species in PM1 and PM10.

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Table 1. Average ratios of indoor and outdoor PM1 and PM10 species. PM10_in/PM10_out PM1_in/PM1_out Average

St. dev.

Average

St. dev.

SO42-

58%

4%

60%

9%

NO3-

19%

4%

19%

9%

Oxalate

52%

7%

54%

9%


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Na+

28%

8%

77%

68%

NH4+

46%

6%

45%

8%

K+

37%

10%

63%

40%

Mg2+

23%

9%

37%

15%

Ca2+

31%

18%

55%

100%

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142 143 144

In the case in which the indoor sources are absent, the average indoor concentrations are lower

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than the outdoor concentrations for all the main species. The average ratio is given by the air

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exchange rate and particle losses during the air exchange and by the strength of the indoor particle

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sink. As all particle losses are size dependent, the compounds present in accumulation mode of the

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particle size distribution (sulfates, oxalates, and ammonium) have similar PM1 and PM10 indoor-

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to-outdoor ratios. Nitrates, although also present in accumulation mode in ambient aerosol, have

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much lower ratios in both size fractions. This result is caused by the dissociation of ammonium

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nitrate indoors, which is driven by a shift in thermodynamic equilibrium caused by nitric acid

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deposition on indoor walls3. The results are similar to those presented in Smolik et al. (2008)4,

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which were obtained at the same location. The differences between the two studies are probably

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caused by differences in meteorological conditions, different types of windows (changed between

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studies), and the installation of a cooker hood with a vent made directly through the wall, which

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changed the ventilation rates.

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Degreaser spray source tests (Using a spray)

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Besides other sources, the W5 degreaser spray was tested twice, first on September 1, 2014, at

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6:30 p.m., second on September 6, at 10:00 a.m. The first experiment is described in detail only as


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very similar results were observed in the second test. The compositional results changed

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substantially after using the degreaser spray (Fig. 2). IC results showed almost complete

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replacement of the NH4+ cation with an mono-ethanol aminium cation (MEA+) both in PM1 (Fig.

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2) and PM10 (Fig. S4). The MEA-containing degreaser W5 was applied 8 h after the beginning of

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sampling. However, almost no NH4+ cation was detected in the sample from this day. Hence, the

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replacement of the NH4+ cation happened not only in the airborne aerosol but also on aerosol

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particles that had been deposited on the filter before the degreaser was applied.

168 169 Before W5 usage

After W5 usage

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Figure 2. Relative equivalent ionic composition of PM1 indoor samples for days with no indoor

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source (21/08 – 31/08) and after using an MEA-containing cleaner (01/09-03/09).

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Fig. 2 contains ion chromatography results for PM1 filters on days when no indoor source was

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present and days after the first usage of the degreaser. (Fig. S4 contains similar data for PM10.)

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The results from the first day, when the degreaser was used, indicate almost complete


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transformation of NH4+ to MEA salts. Despite removing the degreaser from the surface and

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ventilating the room on September 2nd, the partial replacement of NH4+ is observed throughout the

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next few days. This finding seems even more striking if the high air exchange rate 1.26 air

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exchanges per hour is taken into account when the no ventilation experiment was performed27.

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However, the amount of MEA needed for complete replacement of ammonium in the indoor

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aerosol inside small kitchen with 28 m3 volume for 24 hours is actually very small – 2.5 mg of

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MEA. The other aerosol sources examined on September 3rd had no influence on this effect as they

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did not content any MEA.

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Ventilation is expected to cause an exponential decrease in the MEA concentration leading to a

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decrease in concentration by orders of magnitude in the indoor environment; thus, there must have

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remained a weak source of MEA. This source was a leftover on the kitchen surfaces after using a

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paper towel or MEA deposited elsewhere and the paper towel used for cleaning and disposed in

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the kitchen wastebasket. Another possibility is the slow release of MEA from the MEA organic

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salt present in the degreaser.

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Nitrate stabilization

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In addition to the replacement of ammonia in sulfate salts, the replacement of ammonia in

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ammonium nitrate was observed, leading to increased stability and increased concentrations of

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fine nitrates indoors. This conclusion was deduced from almost complete replacement of NH4+ in

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nitrates on September 1st and the differences in the average indoor/outdoor ratio of PM1 nitrate

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concentrations in the period without MEA influence (0.18) and the period with MEA influence

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(0.51). It appears that MEA partially stabilized fine nitrates in the aerosol phase. This effect is also

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shown in Fig. 2 (especially September 1st data) and (less visibly) in Figs. 3 and S5 (AMS data).


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This result agrees with that reported by Salo et al. (2011)11, who measured the evaporation rate of

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aminium nitrate compounds for various amines and found a lower rate of evaporation/dissociation

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for aminium salts of nitric acid relative to ammonium nitrate.

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Time-dependent data

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Using the procedure described above, MEA+ concentrations from the AMS spectra were

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determined. Figs. 3 and S5 shows the real concentrations of ammonium, nitrates, sulfates, and

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organics together with the concentration of MEA+ before and after degreaser usage with

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highlighted time of the degreaser usage. Clearly, the indoor MEA+ salt concentrations were

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elevated immediately after using the degreaser, and this effect persisted for several days in the first

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experiment and until the end of the second experiment (Fig. S5). The organic peak that appeared

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just after using the degreaser spray arose from the aerosolized degreaser solution. Its sharp

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decrease illustrates how standard short-term aerosol emissions behave indoors. In contrast, the

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MEA aerosol concentration remained almost constant until the window was opened before 10 a.m.

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on the next day. This persistence is not possible without interactions that are described above, i.e.

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the evaporation of MEA from a surface followed by the replacement of ammonia in salts present

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in the aerosol.

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The rate of ammonium sulfate transformation to aminium sulfate is strongly depending on

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particle phase as shown by Chu et al. 2017. In our case presence of water in particles may be

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supposed as indoor RH was between 40 and 75%, which favors faster transformation.

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A non-zero concentration of MEA+ was found outdoor via AMS analysis but not on the outdoor

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filter. Although part of the data may represent an artifact connected to the uncertainty of the MEA+

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concentration determination, we cannot exclude the possibility of MEA+ transport to the outdoor


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environment. The differences between the outdoor filter data, where no MEA+ was found, and the

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AMS data can be explained by the fact that the filter samplers are located 5 m from the building,

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which is much farther than the outdoor AMS inlet (0.5 m).

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After the windows were opened, the results significantly changed, but some trends remained. The ammonium appeared again, in salts, but part of the ammonium was still replaced by MEA+.

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Figure 3. Time series of recalculated AMS data indoor (top) and outdoor (bottom) environments

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from the first application of the degreaser at 18:30. At 9:45 on September 2nd, the windows were

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opened for 15 min.

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233 234

Figure 4. Mass size distribution of ionic species on September 2, 2015.

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Similar MEA behavior with the complete replacement of ammonium with indoor MEA+ was also

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observed via AMS during the second experiment when the room was closed throughout the entire

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weekend after the degreaser application at 10 a.m. on September 6th (Fig. S5).

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Cascade impactor results

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In addition to filter sampling and AMS measurement, the BLPI cascade impactor was used on

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September 2nd. An analysis of the samples, shown in Fig. 4, revealed partial replacement of the

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NH4+ cation with MEA+. The mass ratio of MEA+ to the NH4+ ions from impactor stages with

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geometric mean diameters of 0.08, 0.13, 0.20, 0.33, and 0.61 µm were equal to 3.50, 2.02, 1.40,


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0.46, and 0.12, respectively. The size dependence of this ratio, regardless of any uncertainty caused

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by the incomplete separation of the ammonium and MEA+ peaks especially for low values of the

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ratio, clearly shows that the rate of replacement was higher for smaller particles. This finding

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strongly supports the conclusion that the transformation occurred in the aerosol phase and was

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limited by the available surface area.

250 251

Instruments intercomparisons

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To confirm quantitative agreement between the filter samples, impactor samples, and AMS data,

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the approximation of PM1 on the impactor (impactor stages 1-6, stage 6 upper cut diameter of 0.86

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µm) and AMS (AMS total, CE= 0.7 was applied here, see Talbot et al. 201626) were calculated for

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comparison with indoor PM1 filter results on September 2nd.

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The comparison of the data is shown in Table 2 for the major species.

257 258

Table 2. Comparison of concentrations of PM1 aerosol species for different instruments [µg/m3] SO42Leckel PM1 1.53 impactor 1.52 AMS 1.61

NO30.22 0.16 0.23

NH4+ 0.29 0.53 0.19

MEA 0.82 0.26 0.49

259 260

In general, a good agreement was found for sulfates and nitrates. However, MEA+

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concentrations higher than the ammonium cation concentrations were found on the filter, while

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the opposite was true for the cascade impactor. There are two possible causes that have acted in

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conjunction. First, MEA, similar to other organics, have been adsorbed onto the quartz fiber filter;

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thus, part of the analyzed MEA have come from a gas phase. This effect can be deduced from the

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backup filter analysis used for the PM1 filters in which MEA concentrations were found (1-3% of


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the amount found on the front filter), with the maximum on September 1st. Second, the ammonium

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salts already captured on the filter could have reacted with the MEA in the gas phase and increased

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the MEA salt content on the filter. This mechanism could apply to a lesser extent with the impactor

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samples, but only the particles in the upper layer can directly react with the gaseous phase as was

270

observed on the first sampling date when the MEA cleaner was used. This transformation does not

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occur so much on the cascade impactor samples because they are less exposed to the gaseous phase

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relative to particles deposited on a quartz fiber filter. This is also supported by comparison of

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equivalent sum of ammonium and MEA+ for PM1 (30 neqv/m3) and impactor (34 neqv/m3) results

274

that further support this explanation differing within experimental uncertainty. The concentration

275

of MEA found by AMS was in between the filter and the impactor data. The lowest ammonium

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concentration was found using AMS and may be partially artifactual because of the complex

277

corrections applied during the ammonium determination, the indoor environment, and naturally

278

similar MEA fragments.

279 280 281

Implications

282

The use of MEA and other less volatile amine-containing mixtures in our homes and other indoor

283

environments (similar data were found repeatedly in a machinery workshop) significantly changes

284

the chemical composition of indoor aerosols. These changes alter people’s daily interactions with

285

amines, exposing them to various aminium salts that may have unexpected consequences for

286

human health. Moreover, the use of MEA indoors also stabilizes nitrates in the aerosol phase and

287

consequently increases the nitrate exposure to people. The rather insignificant effects of MEA

288

exposure for the general population can be multiplied for professionals working with such


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substances e.g. in restaurants. Therefore, studies on the toxicology of aminium salts, especially

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aminium sulfates and nitrates, on human lungs are needed.

291 292 293

Supporting Information. Text and Figures S1-S3 (PDF)

294 295

Corresponding Author

296

*[email protected]

297

ACKNOWLEDGMENT

298

The authors acknowledge support of this work by the European Union Seventh Framework

299

Programme (FP7/2007e2013) under grant agreement No. 315760 HEXACOMM.

300

SUPPORTING INFORMATION AVAILABLE 

301 302

C-ToF-AMS procedure description for MEA concentration determination including fragmentation table corrections



303 304

Relative equivalent ionic composition of PM10 indoor samples before and after using an MEA-containing degreaser

305



AMS I/O data from the second experiment with MEA containing degreaser

306



I/O EC/OC data from both experiments

307 308

REFERENCES

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