Characteristics and health effects of volatile organic compound emissions during paper and cardboard recycling

Journal Pre-proof Characteristics and Health Effects of Volatile Organic Compound Emissions during Paper and Cardboard Recycling Ramin Nabizadeh, Armin Sorooshian, Mahdieh Delikhoon, Abbas Norouzian Baghani, Somayeh Golbaz, Mina Aghaei, Abdullah Barkhordari

PII:

S2210-6707(19)33546-2

DOI:

https://doi.org/10.1016/j.scs.2019.102005

Reference:

SCS 102005

To appear in:

Sustainable Cities and Society

Received Date:

2 June 2019

Revised Date:

30 November 2019

Accepted Date:

8 December 2019

Please cite this article as: Nabizadeh R, Sorooshian A, Delikhoon M, Baghani AN, Golbaz S, Aghaei M, Barkhordari A, Characteristics and Health Effects of Volatile Organic Compound Emissions during Paper and Cardboard Recycling, Sustainable Cities and Society (2019), doi: https://doi.org/10.1016/j.scs.2019.102005

This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. © 2020 Published by Elsevier.

Characteristics and Health Effects of Volatile Organic Compound Emissions during Paper and Cardboard Recycling

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Ramin Nabizadeha,b , Armin Sorooshianc,d, Mahdieh Delikhoone, Abbas Norouzian Baghania*, Somayeh Golbaza, Mina Aghaeia, Abdullah Barkhordarif a

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Department of Environmental Health Engineering, School of Public Health, Tehran University of Medical Sciences, Tehran, Iran b Center for Air Pollution Research (CAPR), Institute for Environmental Research (IER), Tehran University of Medical Sciences, Tehran, Iran c Department of Chemical and Environmental Engineering, University of Arizona, Tucson, Arizona, USA d Department of Hydrology and Atmospheric Sciences, University of Arizona, Tucson, Arizona, USA e Department of Occupational Health Engineering, School of Public Health, Isfahan University of Medical Sciences, Isfahan, Iran f Department of Occupational Health, School of Public Health, Shahroud University of Medical Sciences, Shahroud, Iran

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*Corresponding author: Abbas Norouzian Baghan; E-mail: [email protected] and [email protected]

Address: Department of Environmental Health Engineering, School of Public Health, Tehran

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University of Medical Sciences, Tehran, Iran

Highlight

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VOC emissions were studied for a waste paper and cardboard recycling factory.

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VOC concentrations reported for multiple factory sections.

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Total HQ for VOCs in recycling processes was more than the acceptable limit.

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LTCRs for VOCs in different sites of PCSWRF ranged from 1.21 × 10−4 to 1.05 × 10−5.

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Exposure indices of VOCs for residents in PCSWRF exceeded the acceptable limit.

Abstract Urbanization generates increased amounts of solid wastes in cities and as a consequence leads to

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high air pollution levels. As a result of these trends, the subject of air quality management for

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sustainable concept of cities has received increasing attention. This work characterized volatile organic compound (VOC) emissions and health effects at different processing stages in a recycling

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facility for waste paper and cardboard. The highest total VOC levels were observed in the conveyor belt line one (5.23 ± 0.33 mg/m3), followed by a baling machine (1.38 ± 0.07 mg/m3), conveyor

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belt line two (1.34 ± 0.08 mg/m3), tipping floor line one (1.22 ± 0.07 mg/m3), and manual

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separation line one (1.20 ± 0.06 mg/m3). Hence, exposure to VOCs lead to high health risks in this PCSWRF, especially at the manual separation stage (HQ = 2.7 - 3 and lifetime cancer risks

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(LTCRs) = 1.11 × 10−4 - 1.03 × 10−4), and strategies such as adjustment of the factory to enclose the conveyors, designing proper ventilation and air conditioning systems, minimization of VOCcontaminated waste generation (pre-treatment), and using personal protective equipment should be considered to eliminate pollutants and to protect workers from the non-carcinogenic and

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carcinogenic effects.

Keywords: Paper and cardboard recycling; Pollution characteristics; VOCs; Carcinogenic and non-carcinogenic; Exposure indices; sustainable

1. Introduction 2

Improper management of municipal solid waste (MSW) in the most cities of developing countries has become a global problem (Shao et al., 2019, Ahmed and Ali, 2004). In addition, the implementation of suitable municipal solid waste management (MSWM) plays a significant role in the sustainable development of cities (Mesjasz-Lech, 2014, Durán and Messina, 2019). Furthermore, rapid urbanization and industrialization generates increased amounts of various solid wastes such as municipal and industrial solid waste (MSW and ISW) in urban areas creating

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thousands of tons of solid waste a day (Ramachandra et al., 2018, Putthakasem et al., 2018,

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Norouzian Baghani et al., 2016, Norouzian Baghani et al., 2017, DES, 2013). Chemical characteristics of these wastes and emissions include hazardous air pollutants that need significant

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resources and infrastructure for minimization of emissions and mitigation of health effects (Durán

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and Messina, 2019). Hence, one of the main factors for attaining the sustainability of cities is rooted in environmental management in the form of waste and recycling management and air

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quality conservation (DES, 2013, Rada, 2014, Heidari et al., 2019). Managing air quality is central to the sustainability of all cities (Maitra, 1998, Rada, 2014, WHO, 2019). On a global perspective,

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not paying attention to this issue promotes major socioeconomic, health, and climate-relevant issues in cities around the world (Rada, 2014, WHO, 2019). A major constituent emitted from such wastes and their processing is volatile organic compounds (VOCs), stemming from sites such as the landfill or processing such as recycling (Urase et al.,

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2008, Sánchez-Monedero et al., 2018, Nie et al., 2018a, Norouzian Baghani et al., 2016, An et al., 2014, He et al., 2015, Palmiotto et al., 2014, Ghosh et al., 2019, Liu et al., 2017). Recycled waste includes paper and cardboard, organic wastes, and plastics, which are the main sources of VOCs in MSW facilities (Komilis et al., 2004, Jackson, 2015, He et al., 2012a, He et al., 2015). Komilis et al. (2004) and Jackson (2015) reported that mixed paper with food waste and fresh waste were

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the main sources of VOCs in landfill and recycled centers, in addition to composting facilities (Jackson, 2015, Komilis et al., 2004). Furthermore, Duan et al. (2014) and Mustafa et al. (2017) reported that the main sources of toluene in solid waste can be papers and cardboard, plastics, and food waste (Duan et al., 2014, Mustafa et al., 2017). Air pollution, especially VOCs, generated from MSW, ISW and waste sorting processing can pose health risks to factory workers and nearby dwellers (He et al., 2015, Li et al., 2013b, Villavert et al., 2009, Gladding and Coggins, 1997,

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Gladding and Gwyther, 2017, An et al., 2014, Dehghani et al., 2018c). Health effects associated

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with exposure to VOCs can be categorized as carcinogenic and non-carcinogenic (Golkhorshidi et al., 2019, Delikhoon et al., 2018a, Dehghani et al., 2018a, Baghani et al., 2018a). In other words,

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exposure to VOCs emitted from solid waste can lead to diseases such as hypochromic anemia,

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headaches, loss of coordination and nausea, respiratory issues, central nervous system problems, allergic skin reactions, emesis, epistaxis, narcosis, fatigue, asthma , dizziness, defatting dermatitis,

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bronchitis, and cancers of the brain, blood, kidney, and lungs (Phillips et al., 1999, Romagnoli et al., 2014, Rumchev et al., 2004, U.S.EPA, 2018, Golkhorshidi et al., 2019, Baghani et al., 2018a,

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Marzouni et al., 2017, Domingo and Nadal, 2009, Hu et al., 2018). For instance, benzene negatively impacts the blood-forming system and contributes to leukemia and hematological disorders and lymphoma cancer (Smith, 2010, Moolla et al., 2015), while toluene impacts the reproductive and neurobehavioral health (Greenberg, 1997, Foo et al., 1990, Tunsaringkarn et al.,

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2012). Generally, the concentration profile of VOCs is a helpful indicator of the potential for harmful effects due to exposure to solid waste emissions (Dehghani et al., 2018b, He et al., 2012a, He et al., 2015, He et al., 2012b). These issues motivate a health risk assessment (HRA) on the workers exposed to VOCs in waste processing facilities. Characterization of VOCs and a HRA of VOCs on the workers in a paper and cardboard solid waste recycling factory (PCSWRF) has yet

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to be performed. Hence, controlling air pollution created by MSW, especially at PCSWRFs, is as important factor for the sustainability of cities and this activity can indirectly impact public health and socioeconomic aspects related to the sustainability of cities (Heidari et al., 2019, Zhu et al., 2019). The goal of this work is to 1) study the concentration of VOCs species in different areas of a

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PCSWRF, 2) identify VOC species and the percentage of VOC species in different areas of a PCSWRF, 3) determine interrelationships between VOCs species and meteorological conditions,

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4) investigate occupational exposure limits (OLE) for workers in different areas of a PCSWRF,

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and 5 ) estimate health risk assessment of workers (carcinogenic and non-carcinogenic) exposure

2. Materials and Methods

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2.1. Descriptions of Study Area

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to VOCs in different areas of a PCSWRF.

This work was carried out in a paper and cardboard solid waste recycling factory (PCSWRF)

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located in Tehran, Iran (35°32'42"N, 51°23'35"E) (Fig. 1). This factory has two lines of separation processes for paper and cardboard, including a tipping floor (line one and two), conveyor belt (line one and two), hand picking/manual separation (line one and two), and finally a baling machine (Fig. 2). Sampling locations were positioned at the tipping floor (line one and two), conveyor belt

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(line one and two), manual separation area (line one and two), baling machine, storage area, office area, and a background area (Fig. 2). Fig. 1. Map of the study area and air monitoring stations.

Fig. 2. A map of operational units (processes units) in the PCSWRF.

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2.2. Sampling and analysis Sampling of VOCs species was carried out based on the U.S.EPA TO-15 method (McClenny and Holdren, 1999, He et al., 2012a, He et al., 2015, Durmusoglu et al., 2010). According to the EPA sampling guideline (EPA, 2006), sampling was carried out every six days from 22 December 2017 to 20 February 2018 using active sampling (SKC 222 Series Low Flow Pump) with a charcoal glass tube at a flow rate of 0.2 L/min for two hours. For the 10 sampling sites (Fig. S1), a total of

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100 VOC samples were collected between December and February. During sampling, the sampler

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was located at breathing zone of the workers (at a height of 1.5 meters above the ground) (Baghani et al., 2018b).

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Seventeen VOCs were examined using gas chromatography–mass spectrometry (GC-MS) (GC

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7890N, AGILENT- MS 5975C, MODE EI.MS), including benzene, toluene, ethylbenzene, m,p xylene, o-xylene, decane, 1-ethyl-3-methyl benzene, 1,2,3-trimethyl benzene, 1,3,5-trimethyl

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benzene, 1,2,4-trimethyl benzene, 1,2-diethyl benzene, 1-ethyl-2-methyl benzene, limonene, 1,4 diethyl benzene, butyl benzene, 2-methyl nonane, and nonane. An HP- 5MS column (60 m × 0.32

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mm × 0.25 μm, Agilent Technologies,USA) was used. Helium was the carrier gas at 1.2 mL per min. The temperature of the GC-MS oven at first was programed to be at 35°C for five minutes, and then increased to 150°C at a rate of 5°C per minute. Finally, the oven temperature reached 250°C at a rate of 15°C per minute and held for two minutes. The MS line delivery line

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temperature, scan mode and ionizing energy were 290°C, 45– 260 (m/e) and 70 eV, respectively. In addition, temperature (°C) and relative humidity (%) were quantified with a portable instrument (Preservation Equipment Ltd, UK and Campbell Scientific, Inc., USA ). 2.3. Quality Assurance/Quality Control (QA/QC)

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In this work, two parts of tubes were analyzed individually for the potential of breakthrough for samples. There were no signs of VOC contamination in the second sections of tube. Six samples were gathered as blank samples and concentrations of VOC species in these tubes were limited to between 0.00 - 0.0032 (µg/m3). A mean recovery of 97% (92-110%) was acquired for VOC species with standard deviations (SDs) less than 5.00%.

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2.4. Statistical Analysis

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Analysis was performed by the statistical program R (version 3.0.1 (2013-05-16)) (Team, 2013). The Fligner-Killeen test was applied to assess for homogeneity of variance. If the p-value obtained

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from the Fligner-Killeen test exceeded 0.05, the ANOVA test was performed for further analysis. But, if the p-value was less than 0.05, the Kruskal-Wallis test was applied for further analysis.

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Furthermore, if the Kruskal–Wallis test was significant, the Kruskal-Wallis post-hoc test (Kruskal

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Mac) was carried out to show that levels of the independent variable vary from other levels. For comparison, VOC concentrations between the two lines of the tipping floor and conveyor belt in the PCSWRF were assessed using the Mann-Whitney-Wilcoxon test, while a paired t-test was used

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for comparison of VOC concentraions between the two lines of manual separation. The relationship between VOC concentrations and meteorological conditions (i.e., temperature, relative humidity) were quantified using Spearman's rho correlation coefficient. In addition,

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occupational exposure indices (Ei) were determined for workers for emitted VOCs in the PCSWRF. In the end, HRA was calculated for estimating the hazard quotient (HQ) and the lifetime cancer risk (LTCR) for VOC species. Figures were drawn using GraphPad Prism 7 and R Statistical Software version 3.0.1. 2.5. Occupational Exposure Limits (OEL) and Health Risk assessment (HRA) for Workers 2.5.1. Occupational Exposure Limits (OEL) 7

According to American Conference of Industrial Hygienists (ACGIH) and International Organization for Standardization (ISO), OELs were determined for humans for some harmful VOC species (Romagnoli et al., 2014, ACGIH, 2001, He et al., 2015). The ACGIH determined threshold limit values (TLV) based on the short-term exposure limit (STEL) and time weighted average (TWA). The Threshold Limit Value-Time-Weighted Average (TLV-TWA) indicates whether an employee's exposure may not surpass the time-weighted average in an eight hour

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workday or forty hour work week (Verma, 2000, Zhang et al., 2018). According to the measured

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VOCs in this work and TLV-TWA in Table S1, the occupational exposure indices (Ei) for emitted

Ei = ∑𝑛𝑖 𝐶𝑜𝑛𝑐𝑒𝑛𝑡𝑟𝑎𝑡𝑖𝑜𝑛𝑠 𝑜𝑓 𝑉𝑂𝐶𝑠 ( 𝑚𝑔 𝑚3

)

𝑚3

) / Threshold limit value − time − weighted average (TLV −

(1)

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TWA) (

𝑚𝑔

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VOCs are determined as follows (He et al., 2015, He et al., 2012b, Mo et al., 2009):

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In this study, Ei > 1 indicates that the potential health risk can be important for the workers in the PCSWRF (Mo et al., 2009, He et al., 2015, He et al., 2012b). According to Mo et al. (2009), it is

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necessary that Ei not exceed the value 1 (Mo et al., 2009). Hence, Ei < 1 demonstrates that the potential health risk cannot be important for the workers in the PCSWRF (Mo et al., 2009). 2.5.2. Health Risk Assessment (HRA)

With regard to the recycling of paper and cardboard performed by workers, it is essential to

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evaluate the carcinogenic and non-carcinogenic health effects of VOCs. In this work, the hazard quotient (HQ) parameter was used for calculating non-carcinogenic health effects of VOCs, which is expressed as the ratio of chronic daily intake (CDI) (mg/kg-day) and the reference dose (RfD) (mg/kg-day) (Table S1) (Delikhoon et al., 2018b, Baghani et al., 2018b, Zhu et al., 2014, Jiang et al., 2018, Shuai et al., 2018, Cao et al., 2018):

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HQ= CDI/ RfD

(2)

Hazard quotients exceeding one (1 ≤ HQ) indicate unsafe risk (harmful health effects) (Durmusoglu et al., 2010, Zhang et al., 2018). In addition, McCarthy et al., (2009), He et al. (2015) and Ramirez et al. (2012) reported that HQ values from 0.1 to 1 still exposes workers to risks (He et al., 2015, McCarthy et al., 2009, Ramírez et al., 2012).

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Furthermore, the lifetime cancer risk (LTCR) was applied to estimate carcinogenic health effects of VOCs, which is specified as the product of chronic daily intake (CDI (mg/kg-day) and cancer

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et al., 2013a, Golkhorshidi et al., 2019, Baghani et al., 2018a):

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slope factor ( CSF (mg/kg-day)-1) (Table S1) using the following equation (Zhang et al., 2018, Li

(3)

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LTCR = CDI (mg/kg-day) × CSF (mg/kg-day)-1) (Table S1)

CDI = (C (pollutant concentrations (µg/m3)) × ET (exposure time (40 h/week or 8 h/days) × EF

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(exposure frequency (48 weeks/year or 240 days/year)× ED (exposure duration (30 year)) × IR (human inhalation rate (0.83 m3/h)) / (BW (body weight (70 kg)) × AT (the average lifetime ((365 (4)

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× 30) 10950 days))

Based on the United States Environmental Protection Agency (U. S. EPA), the IR and BW values for adults are 0.83 m3/h and 70 kg, respectively (Moya et al., 2011, EPA, 2011). According to

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Sexton et al. (2007), Durmusoglu et al. (2010) and Li et al. (2013), if the lifetime cancer risk (LTCRs) exceeds 1 × 10−4, ranges from 1 × 10−5 to 1 × 10−4, is between 1 × 10−5 and 1 × 10−6, or is less than 1 × 10−6, it indicates as definite, probable, possible, and negligible risk, respectively (Durmusoglu et al., 2010, Li et al., 2013a, Sexton et al., 2007). For calculating health risks of VOC species, the equations above were applied separately to compute risks of species and finally the

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risks for all of them combined together. The product of the above equations gave an indication of the total health risk.

3. Results and Discussion 3.1. VOCs Emissions

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In this work, all of locations that included operational units (tipping floor line one and two, baling

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machine, hand picking line one and two, and inclined conveyor belt line one and two), storage, and offices emitted VOCs to the air. The mean concentrations ± (SD) of VOCs emitted from

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operational units, storage areas, office areas, and the outdoor area (background) are described in Table 1. The mean concentrations ± (SD) of TVOCs emitted from PCSWRF were in the following

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order: conveyor belt line one (5.23 ± 0.33 mg/m3) > baling machine (1.38 ± 0.07) > conveyor belt

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line two (1.34 ± 0.08) > tipping floor line one (1.22 ± 0.07) > manual separation line one (1.20 ± 0.06) > manual separation line two (1.06 ± 0.05) > tipping floor line two (0.54 ± 0.02) > office

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(0.69 ± 0.04) > background (0.43 ± 0.02) > storage (0.09 ± 0.01). Among the steps of operational units, inclined conveyor belt one (5.23 ± 1.20 mg/m3) had the most emissions of TVOCs. During the PCSW recycling processes, 17 VOCs were identified and quantified in operational units (Fig. 2). The mean (± SD) concentration of TVOCs (mg/m3) in different operational units is shown in

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Fig. 3. Accordingly, the maximum concentrations of m,p-xylene (1.2 ± 0.11), 1,2,4-trimethyl benzene (0.82 ± 0.05) and 1-ethyl-3-methyl benzene (0.69 ± 0.05) were measured in the conveyor belt line one. In contrast, He et al., (2015) reported that the predominant concentrations of VOCs isolated from the air of in the poly (acrylonitrile-butadiene styrene) (ABS) recycling process in Southern China were styrene (6.3 ± 2.1 × 102 mg/m3), ethylbenzene (1.5 ± 0.5 × 102 mg/m−3), xylene (54 ± 22 mg/m3), toluene (31 ± 14 mg/m3) and i-propylbenzene (28 ± 9 mg/m3) (He et al., 10

2015). In addition, Urase et al. (2008) observed that the main VOCs emitted from the landfill gas into the ambient air were benzene, toluene, ethylbenzene, and xylene (BTEX), trimethyl benzenes and low levels of chlorinated compounds (Urase et al., 2008). Wu et al., (2018) reported that the major VOCs species at MSW landfills in Beijing, China were BTEX, styrene, propylbenzene, naphthalene, and 1,3,5-trimethylbenzene (Wu et al., 2018). Caglia et al. (2011) reported that the main emitted VOCs from MSW in the North Italy were p-xylene, o-xylene, styrene, benzene, 1

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ethyl 4 methyl benzene, 1 methyl 2 (1 methylethyl) benzene, 1 ethyl 4(1 methylethyl) benzene, 1

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methyl 3(1 methylethyl) benzene, 2 ethyl 1,3 dimethyl benzene, 1,2,3 trimethyl benzene, and 1 methoxy 4 methyl 2(1methylethyl) benzene (Scaglia et al., 2011). Hence, the main reasons for

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difference in emitted VOCs from various studies could be explained by differences in sampling

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sites (landfill/disposal, composting, during waste collection, and industrial process), composition of waste (only paper and cardboard or mixed municipal solid waste (MMSW) and thermal

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degradation of different types of plastic wastes (He et al., 2015, Scaglia et al., 2011, Urase et al., 2008, Shen et al., 2018, Pagans et al., 2006). In addition, the findings of this work revealed that

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VOC concentrations in the operational units in the PCSWR ranged between 1.10 ± 0.23 and 5.30 ± 1.20 mg/m3, which is consistent with the results of the previous studies by Lehtinen et al. (2013) in the optic sorting plant in Hämeenlinna and the waste transferring plant in Hyvinkää in Finland (Lehtinen et al., 2013).

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The main VOCs emitted from the processing hall in the optic sorting plant in Hämeenlinna were ethylbenzene, p-xylene, p-cymene, propyl benzene, C3-alkyl benzene, and limonene, each of which ranged between 0.04 to 1.20 mg/m3. The same study showed that the concentrations of limonene (1.20 mg/m3) exceeded other components (Lehtinen et al., 2013), which is in agreement with the findings of the present study. Another study examining urban waste wheel containers for

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VOCs in Athens, Greece showed that the most abundant VOCs included decane, limonen, nonane, and benzene with median concentrations ranging from 212.6 to 694.9 μg/m3 (Statheropoulos et al., 2005). Some VOCs such as styrene, toluene, ethylbenzenes, m,p-xylene, and o-xylene have been emitted from plain paper, especially in the presence of toner, in aged/old books (109 VOCs identified) and processed paper from photocopying machines (Henschel et al., 2001, Betha et al., 2011, Wolkoff et al., 1993, Kumar et al., 2014, Gaspar et al., 2010, Horie, Knight and Horie, 2007,

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Pagans et al., 2006). Furthermore, paper and cardboard production impregnated with oil and grease

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was another source of VOCs (Propst Jr, 2010, Banou et al., 2016, Pagans et al., 2006). Generally, several parameters could lead to emissions of VOCs into the air of operational units in this

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PCSWRF including biodegradation of organic solid wastes, proper moisture content and

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temperatures higher than 30°C in the waste, polystyrene plastic waste, an old ink or toner cartridge, processed paper from photocopying machines, paper and cardboard production impregnated with

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petroleum products, and in old books. The mean concentrations of TVOCs in the indoor microenvironment of the PCSWRF was about 5-19 times higher than indoor microenvironments

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(residential and workplace) in EXPOLIS-Helsinki, Finland (Edwards et al., 2001), and the mean TVOC concentrations in the indoor microenvironment in office of PCSWRF was 19 times lower than in the largest office building in Jahra City since Jahra's large office is located near of oil fields (Al-Khulaifi et al., 2014). In addition, the mean emitted TVOCs in the operational units in

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PCSWRF were 2.5 - 150 times lower than the mean TVOCs concentrations in the melting extrusion process of various plastic solid waste recycling workshops (He et al., 2015). Table 1. The mean ± standard deviation (SD) of VOCs (mg/m3) in different sampling locations in the PCSWRF.

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Fig. 3. The mean (± SD) concentration of TVOCs (mg/m3) in all operational units. 3.2. Frequency of Occurrence of VOCs Species The percentage of measured VOCs during operational units in PCSWRF were in the following order: conveyor belt line one (43.64%) > baling machine (11.55%) > conveyor belt line two (11.22%) > tipping floor line one (10.17%) > hand picking line one (10.01%) > hand picking line

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two (8.88%) > tipping floor line two (4.50%). As mentioned above, the line one was polluted than line two. In addition, the percentage of emitted VOCs in storage, office and background compared

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with operational units were 0.39, 0.77 and 0.12%. Reasons for conveyor belt line one being highest

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in concentration in this work could be linked to proper moisture content and higher temperature as compared to different units, and severe mechanical stirring of solid waste by front-end loaders for

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et al., 2007, Laitinen et al., 2016).

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easier separation of paper and cardboard as compared to manual separation (He et al., 2010, Chiriac

The percentage of detected VOCs based on frequency in different sampling sites were simplified in Fig. S2. As shown in Figs. S2 b and c , the four main species of VOC identified in the indoor

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air of tipping floor (line one vs. line two) were m,p-xylene (21.76 vs. 15.05%), limonene (17.05 vs. 14.51%), 1,2,4-trimethyl benzene (13.80 vs. 12.32%), and toluene (5.65 vs. 13.91%). In addition, according to Figs. S2 d and e , the five dominant species of VOCs in conveyor belt line

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one were m,p-xylene (22.84 %), 1,2,4-trimethyl benzene (15.68 %), 1-ethyl-2-methyl benzene (13.31 %), o-xylene (10.63%), and limonene (9.26%), while in conveyor belt line two the prcentage of these species were 20.52% for m,p-xylene , 11.95% for 1,2,4-trimethyl benzene, 10.74% for 1-ethyl-2-methyl benzene , 8.56% for o-xylene, and 19.61% for limonene. Moreover, Figs. S2 f and g revealed the following differences between line one and line two: m,p-xylene

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(16.64 vs. 10.20%), limonene (14.17 vs. 20.15%), 1-ethyl-2-methyl benzene (12.55 vs. 12.69%), and 1,2,4-trimethyl benzene (11.57 vs. 10.59%). In addition, the results of this work showed that the major pollutants measured in the air of the baling machine were m,p-xylene (19.24%), limonene (15.30%), 1,2,3-trimethyl benzene (11.01%), and 1-ethyl-2-methyl benzene (9.83%) (Fig. S2 h) and the chief reason why the

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concentrations of VOCs were lower than other operational units could be described by the recycled materials (paper and cardboard) were packaged. The main measured VOCs species in storage were

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toluene (66.87%), limonene (12.83%), benzene (7.24%), and 1-ethyl-2-methyl benzene (5.53%)

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(Fig. S2 i). Surprisingly, the percentage of toluene was the first highest VOCs (66.87%) with a mean value of 0.21 ± 0.07 mg/m3, which might be generated by devices such as a liftruck and

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trucks (fresh emissions) during loading bales and waste materials that includes VOCs (fresh waste/ mixed paper with food wastes) (Dehghani et al., 2018b, Termonia and Termonia, 1999, Hoque et

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al., 2008, Chiriac et al., 2007, Conte et al., 2018, Nie et al., 2018b, Komilis et al., 2004, Jackson, 2015). The major VOCs emission from the office building included m,p-xylene (24.52%), toluene

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(15.61%), benzene (10.88%), and o-xylene (6.84%), while the main VOCs emitted in ambient background air (outdoor) were m,p-xylene (19.19%), limonene (14.81%), toluene (14.25%), and 1,2,3-trimethyl benzene (8.13%) (Figs. S2 j and a). For contrast, the findings of this work were opposite to other studies in that the main VOCs discharged into the air of plastic solid waste

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recycling workshops (PSW) with pyrolysis of plastics were BTEX and styrene (He et al., 2015, Mehta et al., 1995). In this work the main factors leading to emisions of VOCs into the air were the materials that included VOCs (fresh waste and mixed paper with food wastes) and some processes such as fermentation of paper and cardboard (Zhu et al., 1998, Arshadi and Gref, 2005, He et al., 2010, Gaspar et al., 2010, Komilis et al., 2004, Jackson, 2015), while the main source of

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discharged VOCs into the air of PSW workshops was thermal degradation of different types of plastics at high tempreture (more than 160°C) (He et al., 2015, Mehta et al., 1995). Generally, the main species of VOCs in the different processes of the indoor microenvironment were m,p-xylene, limonene and 1,2,4-trimethyl benzene. Furthermore, the predominant VOC species in the PCSWRF were m,p-xylene, limonene, 1,2,4-trimethyl benzene, 1-ethyl-3-methyl

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benzene, and toluene. Finally, the VOC concentrations decreased from the tipping floor to the

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baling machine, and were lowest in the storage site. 3.3. Statistical Analysis of VOCs in PCSWRF

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3.3.1. Interrelationships Between VOCs Species and Meteorological Conditions

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Table S2 summarizes Pearson's correlations among VOC concentrations based on mean concentrations and meteorological parameters for all sites in the PCSWRF. Accordingly, the

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correlation coefficients (r) for VOC species in most places of the PCSWRF were higher than 0.679. In addition, significant positive correlations were among among VOCs species. These results

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showed that VOC species had similar sources and the recycled materials that included VOCs (fresh waste and mixed paper with food wastes) were the major sources of VOCs in the PCSWRF (Komilis et al., 2004, Jackson, 2015). The maximum correlation coefficient (r = 0.999, p < 0.01) was obtained between 1,2,3-trimethyl benzene and 1,4-diethyl benzene.

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A significant correlation was observed between VOCs species with either relative humidity or temperature (p < 0.01) except for benzene, toluene, ethylbenzene, and nonane. Hence, the results of this work shows that concentrations of VOC species were not related to fresh emissions except for storage site where liftruck and trucks (fresh emissions) can generate VOCs species. In general, these findings are highly indicative of the recycled materials that include VOCs species (fresh

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waste and mixed paper with food wastes) as the main source of VOCs species in the air of PCSWRF. 3.3.2. Statistical Analysis of VOCs in Different Sampling Location Fig. S3 displays a box plot of VOC concentrations in different sampling locations (storage, office, process and background). The output of the Fligner-Killeen test showed that p-value for VOC

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concentrations in different sampling stations was lower than 0.05 (p < 0.05). This indicates that the difference between the variances in different processes were significant (p < 0.05). Therefore,

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analysis of variance was used to compare normally distributed variables for more than two groups

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(Kruskal-Wallis test). The results of the Kruskal-Wallis test on VOC concentrations in different sampling stations was significant at a level of 0.05. Consequently, the results of the Kruskal-

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Wallis post-hoc test (Kruskal Mac) showed that the mean concentrations of VOCs between two different sampling locations of background – storage, background - process and office – storage

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were significantly different (p < 0.05).

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3.3.3. Statistical Analysis in Different Processes

The results of the Mann-Whitney-Wilcoxon test showed that there was no statistically significant difference between VOC concentrations in tipping floor line one and two (p ≤ 0.001) and conveyor belt line one and two (p ≤ 0.001), while the results of the paired t-test showed that a

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statistically significant difference was observed between concentrations of VOCs in manual separation line one and two (p = 0.112). Hence, VOCs concentrations of manual separation line one and two were combined together as a defined manual separation line (Fig. 4). Box plot of VOCs concentrations based on mg/m3 in different processes (operational units) is shown in Fig. 4. Accordingly, the output of the Fligner-Killeen test showed that p-value for VOCs in different processes (tipping floor line one and two, conveyor belt line one and two, manual separation line, 16

and baling machine) was lower than 0.05 (p < 0.05). This indicates that the difference between the variances in different processes were significant (p < 0.05). Therefore, analysis of variance was used to compare normally distributed variables for more than two groups (Kruskal-Wallis test). Hence, the results of Kruskal-Wallis test on VOCs concentrations in different processes described that the chi-square test statistic was 14.45, which was significant at a level of 0.05. Therefore, it is safe to say that there were significant difference between the concentration of VOCs in different

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operational units (p < 0.05). Consequently, the results of the Kruskal-Wallis post-hoc test (Kruskal

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Mac) showed that the mean concentrations of VOCs between two different operating units of baling machine - tipping floor line two, conveyor belt line one - conveyor belt line two , conveyor

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belt line one - manual separation line, conveyor belt line one -tipping floor line one, conveyor belt

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line one - tipping floor line two, and manual separation line -tipping floor line two were significantly different (p < 0.05).However, there was not a significant difference between the mean

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concentrations of VOCs in other operating units (p > 0.05).

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Fig. 4. Box plot of VOC concentrations in different processes (operational units) in winter. 3.4. Occupational exposure limits (OEL) assessment for workers in PCSWRF VOCs with high levels could lead to chronic and acute health effects for those in the PCSWRF.

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Therefore, based on emitted VOCs, we can calculate occupational exposure limits (OEL) for the workers. A threshold limit value-time-weighted average (TLV-TWA) of 10 out of 17 measured VOCs were valuated for health effects of the workers in this work (Table S1). According to TWA– TLV the exposure indices (Ei) for 10 emitted VOCs from the PCSWRF in different sites are shown in Fig. S4. As can be seen, the Ei for TVOCs in all of sites in PCSWRF were higher than one except for the background and storage areas. This indicates that people in this factory might suffer 17

from health effects of VOCs from different sites and that workers should pay attention to the health effects of VOCs. Moreover, the highest sum of Ei for TVOCs in this work revealed the following order of abundance: hand picking line two (4.5) > conveyor belt line one (4.2) > hand picking line one (3.5) > hand picking line one (3.8) > conveyor belt line two (3.1) > tipping floor line one (1.9) > tipping floor line two (1.7) > baling machine (1.1) > background (0.63) > storage (0.45). In this work, benzene with the highest average Ei of 3 accounted for more than 85% of

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TVOC Ei in the PCSWRF since TLV-TWA for benzene (1.7 × 10-3 mg/m3) was lower than the

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other compounds (Table S1). The the mean Ei of nonane (TLV-TWA = 1.1 × 103 mg/m3) was lower than 0.001, and accounted for lower than 0.002% of TVOC Ei. In addition, the mean Ei of

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TVOCs for background and storage areas were lower than one. Generally, the Ei for TVOCs in

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different sites was more than one, and so using personal protective equipment (PPE) such as respirators and gloves can help workers decrease exposure to emitted VOCs in this WPCRF.

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3.5. Health Risk Assessment (HRA) for VOCs

All of 17 measured VOCs were evaluated based on the RfD values for non-carcinogenic effects

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(Table S1). According to concentrations of VOCs (Table 1), the HQ of VOCs are summarized in Fig. S5. The highest sum of HQs with a value of 5.8 for the examined VOCs was acquired in the conveyor belt line one, followed by hand picking line two (3), hand picking line one (2.7),

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conveyor belt line two (2.6), office (1.6), tipping floor line one (1.1), baling machine (0.88), tipping floor line two (0.72), background (0.64), and storage (0.17). With the HQ more than one, noncarcinogenic risk could be introduced to the workers by VOCs discharged from the conveyor belt line one, where the top three compounds for HQs were 1,3,5-trimethyl benzene (1.78), nonane (1.4) and benzene (1.06), accounting for 30.79%, 23.48% and 17.56% of the cumulative HQ, respectively. Furthermore, the HQ of conveyor belt line one was two times higher than line two so 18

the non-carcinogenic risk of line one is two times larger than line two. In the conveyor belt line two, the only compound that affects non-carcinogenic risk of workers was nonane (HQ = 1.29), which supports the 48.98% of total hazard quotient (2.6). In addition, the HQs for manual separation line two exceeded one, representing a non-carcinogenic risk for residents; benzene (41.22 to 42.91%) and nonane (34.74 to 36.38%) had the highest HQs for line two. Moreover, the total HQs in the office area was 1.6 and benzene is the main pollutant that the residents were

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exposed to (HQ = 1.18), contributing 75.14% of the total non-cancer risk. As for the other sites,

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the total HQ was lower than one, indicating a non-carcinogenic risk of VOC species.

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McCarthy et al., (2009), He et al. (2015) and Ramirez et al. (2012) reported that HQ values from 0.1 to 1 could make the site workers vulnerable to health risks (He et al., 2015, McCarthy et al.,

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2009, Ramírez et al., 2012). The HQs for benzene in the indoor microenvironments of the PCSW such as tipping floor line two, conveyor belt line two, manual separation (line one and two),

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background, baling machine, and storage ranged from 0.1 to 0.73, describing 24 to 65% of the total non-carcinogenic risk. Furthermore, 1,3,5-trimethyl benzene (HQs = 0.13 to 0.34) also

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accounted for 8.31 to 18.11% of the sum non-carcinogenic risk in the indoor air of tipping floor line one, conveyor belt (line two), hand picking (line one and two), and baling machine. Furthermore, 1,2,4-trimethyl benzene (HQs = 0.1 to 0.73) contributed 3.36 to 12.7% of the total HQs of PCSW recycling factory, especially for indoor air of tipping floor line one, conveyor belt

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(line one and two), hand picking (line one and two). Moreover, the HQ for 1,2,3-trimethyl benzene was limited between 0.19 and 0.23, which contributes 4 to 21.8% of the total HQ of VOCs for the PCSW recycling factory, especially for indoor air of conveyor belt line one and baling machine. Finally, in the indoor microenvironment of conveyor belt line one, o-xylene was also the main non-carcinogenic risk for residents (estimating for 3% of total HQs) with the HQ of 0.17. Based

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on the International Agency for Research on Cancer (IARC), two of the measured VOCs were benzene (group 1) and ethylbenzene (group 2B) that are categorized as a human carcinogen and probable human carcinogen, respectively (Dehghani et al., 2018b, Lim et al., 2014, IARC, 2014). Fig. S6 describes the LTCRs of the carcinogenic VOCs in PCSWRF. The highest total of LTCRs (1.21 × 10−4) occurred in the indoor microenvironment of the office, followed by manual separation line two (1.11 × 10−4), manual separation line one (1.03 × 10−4), conveyor belt line one

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(9.74 × 10−5), conveyor belt oute two (7.64 × 10−5), tipping floor line one (5.06 × 10−5), tipping

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floor line two (4.19 × 10−5), baling machine (3.02 × 10−5), background (1.51× 10−5), and storage (1.05× 10−5). It should be noted that the workers in the office and manual separation process (line

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one and two) of the PCSW recycling factory have been exposed to cancer risks. In the former three

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sites, the total of LTCRs was mostly provided by benzene (participating for 92.24%, 92.30% and 85.12% of the sum of LTCRs, respectively) whose LTCRs values transcended a level of 1 × 10 −4

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(Durmusoglu et al., 2010, Sexton et al., 2007, Li et al., 2013b). Besides, LTCRs for ethylbenzene in office, manual separation line one and two were calculated, respectively 9.38 × 10−6 (7.76% of

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total LTCRs) , 8.56 × 10−6 (7.70% of total LTCRs) and 1.53 × 10−5 (14.88% of total LTCRs). Durmusoglu et al. (2010) reported that compounds with LTCRs from 1 × 10−5 to 1 × 10−6 can be categorized as a “possible risk” (Durmusoglu et al., 2010), which is ethylbenzene in this work. Li et al. (2013) reported that ethylbenzene (8.95 × 10−6), dichloropropane (9.50 × 10−6) and

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trichloromethane (7.36 × 10−6) discharged from the MSW compression transfer station during periods when the compressor was working were identified as a “possible risk” (Li et al., 2013b). In addition, in plastic solid waste recycling workshops (PSW) in southern China, 1,2dichloromethane was a probable risk for workers with LTCR more than10−5 (contributing 51.5 to 55.9% of the LTCR) (He et al., 2015). Furthermore, the study by Ramírez et al. (2012) in the

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ambient air of a large Mediterranean industrial site showed that ethylbenzene (3.5 × 10−6) and tetrachloroethylene (2.3 × 10−6) were identified as a probable risk for workers (Ramírez et al., 2012). Finally, benzene (Group 1) and ethylbenzene (group 2B) can promote cancers such as those of the brain, lungs, liver, and kidneys for workers at office, manual separation line one and two in PCSWRF, which is consistent with former findings (Huff et al., 2010, He et al., 2015, Lehtinen et al., 2013, Durmusoglu et al., 2010). Hence, exposure to VOCs leads to high risk in the PCSWRF,

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especially at hand picking line two (HQ = 3 and LTCRs = 1.11 × 10−4), hand picking line one (HQ

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= 2.7 and LTCRs =1.03 × 10−4), office (HQ = 1.6 and LTCRs = 1.21 × 10−4) and strategies should be considered to eliminate pollutants and to keep workers immune from the non-carcinogenic and

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carcinogenic effects.

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3.6. Control Methods for VOCs

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The different levels of VOCs are released from various municipal waste management practices such as recycling, composting, incineration, and landfilling (Zhaoa et al., 2017, Sarkhosh et al., 2017). Controlling VOC emissions from waste paper and cardboard recycling factories is

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important for the sake of improving the general health of workers and inhabitants in locations with these operations, in addition to improving air quality. Generally, current VOCs control strategies at PCSWRFs can be categorised into three methods including pre-treatment (reduction) of VOC-

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contaminated waste, and also in situ and post-treatment methods (Shen and Sewell, 1988). With pre-treatment methods such as steam-stripping, air-stripping, and carbon adsorption, VOCs can be eliminated from paper and cardboard before it enters to the PCSWRF (Li et al., 2018, Babar and Shareefdeen, 2014). In addition, separation of paper and cardboard production impregnated with oil and grease, especially at tipping floor sites, can reduce emissions of VOCs in PCSWRF (Propst Jr, 2010, Banou et al., 2016, Pagans et al., 2006). In situ control methods commonly include 21

collection and removal systems (Shen and Sewell, 1988). These methods commonly contain enclosures and covers for most of the treatment facilities. Post-treatment methods commonly include tools of gathering VOCs from wastes, especially at storage site sin PCSWRFs by using a cover, vent, and unit of carbon absorption (Shen and Sewell, 1988). Designing proper ventilation and air conditioning systems can help workers decrease exposure to

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emitted VOCs in PCSWRFs (Liu et al., 2017). The present study motivates the need for VOC emission control strategies concentrated on either pre-treatment or post-treatment, which can

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definitely decrease the concentrations of VOCs and be feasible and cost-effective strategies, which

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is consistent with the results of the previous studies (Shen and Sewell, 1988, Banou et al., 2016, Propst Jr, 2010).

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4. Conclusions

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This study concentrated on characterizing the health effects and concentrations of VOCs in the atmospheric air of paper and cardboard solid waste recycling factory (PCSWRF) of Tehran, Iran.

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The conveyor belt line one generated especially significant levels of VOCs. The mean concentrations ± (SD) of TVOCs emitted from PCSWRF were in the following order: conveyor belt line one (5.23 ± 0.33 mg/m3) > baling machine (1.38 ± 0.07) > conveyor belt line two (1.34 ± 0.08) > tipping floor line one (1.22 ± 0.07) > manual separation line one (1.20 ± 0.06) > manual

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separation line two (1.06 ± 0.05) > tipping floor line two (0.54 ± 0.02) > office (0.69 ± 0.04) > background (0.43 ± 0.02) > storage (0.09 ± 0.01).The main species of VOCs in the different processes of PCSWRF were m,p-xylene, limonene, 1,2,4-trimethyl benzene, 1-ethyl-3-methyl benzene, and toluene. The exposure indices (Ei) revealed that the workers can suffer from acute and chronic health effects in the recycling of paper and cardboard factory. These results showed that VOC species had similar sources and the recycled materials that contained VOCs (fresh waste 22

and mixed paper with food wastes) were the major sources of VOCs in the PCSWRF. Noncarcinogenic hazard quotient (HQ) in processes of recycling were more than 1.1, posing a chronic health effect threat for workers. The LTCRs for VOCs in the studied PCSWRF were higher than 1 × 10−4, indicating a definite cancer risk for workers. As Ei and HQ for VOCs in almost all of the sites exceeded one, usage of personal protective equipment (PPE) such as respirators and gloves, designing proper ventilation and air conditioning systems, and minimization of VOC-

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contaminated waste generation (pre-treatment), can help workers decrease exposure to emitted

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VOCs in these types of facilities.

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Declaration of interests

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The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

Conflict of Interest:

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The authors declare that they have no conflict of interest. References

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Fig. 1. Map of the study area and air monitoring stations.

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Fig. 2. A map of operational units (processes units) in the PCSWRF.

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Fig. 3. The mean (± SD) concentration of TVOCs (mg/m3) in all operational units.

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Fig. 4. Box plot of VOC concentrations in different processes (operational units) in winter.

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Table 1. The mean ± standard deviation (SD) of VOCs (mg/m3) in different sampling locations in the PCSWRF. Manual separation line two 0.070±0.008

Baling machine

Storage

Office

Background

0.047±0.004

Manual separation line one 0.059±0.004

0.065±0.009

0.017±0.001

0.007±0.001

0.076±0.005

0.010±0.001

0.075±0.008 0.008±0.001 0.078±0.006 0.033±0.003 0.014±0.002 0.013±0.002

0.095±0.007 ND 1.195±0.118 0.557±0.047 0.184±0.023 0.687±0.049

0.073±0.008 0.031±0.002 0.276±0.023 0.116±0.014 0.030±0.002 0.145±0.020

0.078±0.010 0.066±0.006 0.200±0.014 0.096±0.011 0.036±0.004 0.151±0.011

0.071±0.006 0.037±0.003 0.109±0.011 0.056±0.005 0.025±0.003 0.135±0.012

0.106±0.010 0.021±0.002 0.267±0.030 0.124±0.016 0.054±0.007 0.036±0.005

0.065±0.005 0.011±0.001 0.012±0.002 0.011±0.001 0.011±0.001 0.005±0.001

0.106±0.010 0.040±0.005 0.171±0.014 0.048±0.005 0.015±0.001 0.079±0.008

0.061±0.005 0.003±0.000 0.082±0.010 0.027±0.003 0.016±0.001 0.010±0.001

0.034±0.004

0.041±0.005

0.187±0.018

0.027±0.002

0.032±0.004

0.028±0.003

0.153±0.017

0.011±0.001

0.015±0.001

0.035±0.005

0.045±0.004 0.168±0.017 ND 0.018±0.002

0.013±0.001 0.067±0.009 0.011±0.001 0.010±0.001

0.286±0.023 0.821±0.094 0.081±0.007 0.201±0.023

0.035±0.004 0.161±0.018 0.065±0.007 ND

0.044±0.006 0.139±0.010 0.014±0.001 0.038±0.005

0.055±0.004 0.113±0.011 0.013±0.001 0.036±0.003

0.025±0.002 0.028±0.002 ND 0.136±0.013

0.011±0.002 0.012±0.001 ND 0.013±0.002

0.021±0.002 0.071±0.008 ND 0.015±0.001

0.011±0.002 0.013±0.001 0.034±0.003 0.008±0.001

0.265±0.019 0.034±0.004 0.031±0.003 0.011±0.001 ND 1.220±0.079

0.081±0.010 0.041±0.004 0.014±0.002 0.005±0.002 0.008±0.003 0.541±0.027

0.485±0.034 0.187±0.021 0.184±0.014 0.013±0.001 0.007±0.001 5.234±0.335

0.264±0.026 0.027±0.002 0.030±0.003 0.013±0.001 0.006±0.002 1.346±0.086

0.170±0.012 0.032±0.004 0.036±0.005 0.005±0.002 0.005±0.003 1.202±0.060

0.215±0.021 0.038±0.004 0.051±0.006 0.009±0.001 0.006±0.001 1.066±0.054

0.212±0.027 0.153±0.017 0.054±0.005 ND ND 1.386±0.078

0.012±0.001 0.014±0.003 ND ND ND 0.097±0.018

0.012±0.001 0.015±0.001 0.015±0.001 ND ND 0.696±0.047

0.064±0.005 0.035±0.004 0.016±0.002 0.008±0.003 0.003±0.002 0.430±0.024

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Conveyor belt line two

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1,3,5-trimethyl benzene 1,2,4-trimethyl benzene 1,2-diethyl benzene 1-ethyl-2-methyl benzene Limonene 1,4-diethyl benzene Butyl benzene 2-methyl nonane Nonane TVOCs ND - Not Detectable

Conveyor belt line one

ro

Toluene Ethylbenzene M,P-xylene O-xylene Decane 1-ethyl-3-methyl benzene 1,2,3-trimethyl benzene

Tipping floor line two 0.027±0.003

-p

Benzene

Tipping floor line one 0.030± 0.004 0.069±0.005 0.030±0.003 0.208±0.018 0.095±0.011 0.031±0.003 0.152±0.021

re

pollutant

34