Effect of source-classified and mixed collection from residential household waste bins on the emission characteristics of volatile organic compounds

Effect of source-classified and mixed collection from residential household waste bins on the emission characteristics of volatile organic compounds

STOTEN-135478; No of Pages 9 Science of the Total Environment xxx (xxxx) xxx Contents lists available at ScienceDirect Science of the Total Environm...

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STOTEN-135478; No of Pages 9 Science of the Total Environment xxx (xxxx) xxx

Contents lists available at ScienceDirect

Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv

Effect of source-classified and mixed collection from residential household waste bins on the emission characteristics of volatile organic compounds Xiaoxiao Shi, Guodi Zheng ⁎, Zhuze Shao, Ding Gao Center for Environmental Remediation, Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China

H I G H L I G H T S

G R A P H I C A L

A B S T R A C T

• VOCs released from dustbins by using two collection methods were measured. • The concentration of VOCs emitted from the dustbins reduced after classification. • The OFP of VOCs reached the highest value in summer (1.02 × 103 μg/m3). • The cumulative risks of VOCs exceeded unacceptable levels in spring and summer.

a r t i c l e

i n f o

Article history: Received 8 September 2019 Received in revised form 7 November 2019 Accepted 9 November 2019 Available online xxxx Keywords: Municipal solid waste Volatile organic compounds Classified collection Mixed collection Health risk assessment Ozone formation potential

a b s t r a c t The implementation of domestic waste classification following the principles of reduction, recycling, and harmlessness is an effective method to improve the urban and rural environments and to promote resource recycling. However, in many developing countries, the community residents lack awareness of the benefits of classified collection, which leads to a lack of initiative to classify MSW. To make the people realize the importance of MSW classification and increase the classification dynamics, Suzhou, China was taken as an example in this study, and residential areas were selected as sampling sites for classified and mixed collection of domestic waste. The main components of the odorous volatile organic compounds (VOCs) emitted from the dustbins via different disposal modes were determined by sampling in spring, summer, autumn, and winter. In addition, the ozone formation potential (OFP) and human health risk assessment of the VOCs were analyzed. Halogenated compounds were the major pollutants from the household waste dustbins of the residential areas. However, aromatic compounds contributed the most to the OFP of the VOCs. The OFP of VOCs reached the highest peak in summer, which was 1.02 × 103 μg/m3. Furthermore, more attention needs to be paid in classifying waste to reduce the concentration of OFP. Although there was a carcinogenic risk in spring and summer, it declined after waste classification. Compared with mixed collection, the source-classified collection of garbage had advantages in terms of controlling the emission of VOCs, ozone formation potential, and human health risk. These results could provide the evidence demonstrating the advantages of waste classification and attract people's attention. Furthermore, the results can also provide impetus to those countries, where separate collection of waste has not yet been implemented, to improve the enthusiasm for classification and the integrity of waste classification system. Residents should be encouraged to classify household waste in residential areas. © 2018 Elsevier B.V. All rights reserved.

⁎ Corresponding author at: Center for Environmental Remediation, Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China. E-mail address: [email protected] (G. Zheng).

https://doi.org/10.1016/j.scitotenv.2019.135478 0048-9697/© 2018 Elsevier B.V. All rights reserved.

Please cite this article as: X. Shi, G. Zheng, Z. Shao, et al., Effect of source-classified and mixed collection from residential household waste bins on the emissi..., Science of the Total Environment, https://doi.org/10.1016/j.scitotenv.2019.135478

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1. Introduction

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With the acceleration in urbanization and the improvement of living standards, the amount of municipal solid waste (MSW) is increasing yearly. The International Energy Agency claimed that the worldwide production of MSW was approximately 1.30 × 109 metric tons in 2013. It is expected to reach 2.70 × 109 metric tons by 2050 (IEA, 2016). With the increasing MSW production, the burden on follow-up waste treatment facilities will also increase; still, domestic waste sorting will be conducive to subsequent treatment processes. Many developed countries have successfully implemented waste classification since the late 20th century (Han and Zhang, 2017). For instance, in the United States, the total treatment requirement for MSW decreased by 34.5% in 2012 after classification (EPA, 2014). Similarly, in Germany, the domestic waste recycling ratio increased from 10% in 1980 to more than 40% in 2007 (Zhang et al., 2010). In Singapore, 7.69 × 106 metric tons MSW was generated, of which 60% was recycled, and the disposal capacity requirement decreased to 3.06 × 106 metric tons in 2018 (NEA, 2018). Standardized waste sorting collection systems and high waste recycling rates were implemented to reduce the amount of waste disposal in these developed countries. However, in most developing countries, MSW management institutions are not well managed (Cetrulo et al., 2018), and classified collection systems are not ideal (Blackman et al., 2013). For example, in India, the amount of waste generated in 2015 was approximately 1.43 × 105 metric tons/d. However, MSW is separated at the source only in some areas such as Puducherry (Pattnaik and Reddy, 2010). China's waste sorting system has not been fully implemented owing to underdeveloped facilities (Wang, 2012) and a lack of corresponding regulations and sanctions (Zhuang et al., 2008; Yu, 2013; Han and Zhang, 2017). Mixed collection of garbage wastes resources and causes serious environmental pollution problems (Guo et al., 2017). Odor pollution is one of the most serious problems and often complained about by local residents; it also affects the local environmental quality and disturbs the surrounding residents (Palmiotto et al., 2014; Tan et al., 2017; Cheng et al., 2019). Odor pollution usually refers to an unpleasant smell that is caused by one or more volatile organic compounds (VOCs), usually at a low concentration. Ethanethiol is one such example that can emit a strong odor in the air even at small concentrations of only a few ppb (Kim et al., 2007) and humans or other animals can detect its presence through olfactory perception. Except for NH3 and H2S, odor pollution is mainly caused by VOCs generated through the aerobic or anaerobic fermentation of biodegradable organic matter in piled garbage (Scaglia et al., 2011). Therefore, VOCs can be considered the major air pollutants owing to their odor and dangerous characteristics. In addition, VOCs and strong oxidizing substances in the atmosphere (e.g., OH•) can cause photochemical reactions and produce less volatile oxidation products, which can oxidize NO to NO2, and the produced NO2 can be converted into secondary pollutants, such as ozone, which is the main pollutant responsible for the formation of photochemical smog (Sheng et al., 2018). VOCs can lead to global warming, stratospheric ozone depletion, tropospheric ozone formation (Durmusoglu et al., 2010), and serious environmental health problems (Chu et al., 2019). Long-term exposure to VOCs can cause neurasthenia, respiratory tract damage, central nervous system damage, and increased cancer risk (Domingo et al., 2015; Tong et al., 2019). Especially in children, exposure to air pollution can increase asthma and respiratory diseases because of their developing lungs and immune systems (Labelle et al., 2015; Brand et al., 2016). Many scholars have studied the environmental impact of VOCs in waste treatment facilities such as transfer stations, landfills sites, and composting plants (Fang et al., 2012; Liu et al., 2016; Guo et al., 2017; Nie et al., 2018). However, the hazards of VOCs in the community waste bins have not been considered. Especially in developing countries, district garbage classification systems are not completely ready; on the other hand, the degree of resident participation is not high and the environmental impact of garbage classification is not clearly understood. To help people realize the importance of waste classification and

increase the classification dynamics, the impact of the collection methods on the amount of VOC released needs to be studied. Besides, the importance of waste classification can be proved from the perspective of environmental protection and human health risk. This study selected the largest developing country, namely China, and used Suzhou as a case study (with an urbanization rate of 76.05% by 2018) to measure the concentration of VOCs emitted from the classified and mixed collection bins. In addition, considering the environmental and health impacts, the ozone formation potential OFP and health risks of the VOCs were compared and discussed. The results will provide a theoretical basis for the classification of residential waste and improvement of the waste classification system. 2. Materials and methods 2.1. Sampling site and method In Suzhou, China, kitchen waste bins and other household waste bins in the waste sorting community and mixed household waste bins in the mixed collection community were sampled. The sampling time was chosen as 12:00 am and 6:00 pm before the transportation of domestic waste, and each sample was obtained three times. In each waste bin, six samples were selected for analyzing the concentration of VOCs. The sampling time and environmental factors are shown in Table 1. Gas samples were collected by using the negative pressure method, and the sampling device comprised a sampler and a sampling bag (Zhu et al., 2016; Nie et al., 2018). The sampler consisted of a lung sampling tank, sampling gun, and vacuum pump. 2.2. Analysis method To reduce any error caused by a long interval between the sampling and analysis, considering the high reactivity of the VOCs, a HAPSITE ER portable gas chromatograph-mass spectrometer (US INFICON) was used to analyze the collected gas samples on site. The precision and accuracy of portable gas chromatography–mass spectrometry systems are slightly lower than those of large desktop instruments, but still meet the analysis requirements (Lv et al., 2010). Before being used, the instrument was calibrated using TO-15 mixed standard gas (64 substances), PAMs mixed standard gas (57 substances), sulfide mixed standard gas (5 substances), and terpene mixed standard gas (3 substances). The calibration function of ER-IQ software was used to analyze the standard gas spectrum, and the standard curve and regression equation were integrated into the analysis method file from the analysis results, and then imported into the built-in storage of the instrument through wireless transmission. Such devices have been used by many environmental monitoring departments, research institutes, and military agencies in China and abroad for daily as well as emergency testing (Xu et al., 2011; Harshman et al., 2015; Nie et al., 2019). 2.3. Ozone formation potential analysis methods The methods employed to define the chemical reactivity of VOCs mainly include propylene equivalent concentration and maximum incremental reactivity (MIR) scale (Chameides et al., 1992; Carter, 1994; Venecek et al., 2018). In this study, MIR was used to compute the contribution of VOCs to the OFP (Chen and Luo, 2012; Wang et al., 2018a,

Table 1 Environmental parameters of sampling points. Time

Average temperature (°C)

Average humidity (%)

Spring (April) Summer (July) Autumn (October) Winter (December)

24.9 32.6 23.9 10.0

55 59 65 35

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2018b; Tohid et al., 2019). The calculation of OFP can be expressed by the following formula: C OFP ¼ C VOC  K MIR

ð1Þ

Here, COFP is the OFP of VOCs, CVOC is the ambient concentration, and KMIR is the coefficient of the OFP referring to the MIR. This study adopted the coefficient of VOCs from Carter's findings (Carter, 1994, 2009).

3

600 Spring

Summer

Autumn

Winter

500 Terpenes Sulfuric compounds Aromatic compounds Halohydrocarbons Alkanes Total-MC Total-KW Total-O

400

300

2.4. Human health risk assessment 200

Health risk is based on the risk as an evaluation index and on the quantitative or qualitative analysis of the risk of environmental pollutants to human health. The health risk assessment was divided into non-carcinogenic risk (also termed hazard relation; HR) and carcinogenic risk (CR) assessment on the basis of the carcinogenic potential of the pollutants. In this study, the EPA-540-R-070-002 method was used to assess the health risks of the VOCs in the environment. This study assessed the HR by calculating the exposure risk value and the CR by calculating the lifetime risk. The specific calculation method is as follows: ðC  DET  EF  EDÞ EC i ¼ air AT  365  24  1000 HR ¼

EC i RFC

CR ¼ ðEC i  IUR  1000μg=mg Þ

ð2Þ ð3Þ ð4Þ

Here, ECi is the exposure concentration of each compound (μg/m3), Cair is the emission concentration for each volatile compound in ambient air (g/m3), DET is the daily exposure time (1 h/d in this study), EF is the exposure frequency (350 d/y), ED is the exposure duration (30 y), and AT is the average time, namely 25 y for HR and 70 y for CR. The HR was calculated using Eq. (3), in which RFC represents the reference concentration (mg/m3). Meanwhile, the CR was calculated using the inhalation unit risk (IUR) (μg/m3) given in Eq. (4). The RFC and IUR values from the California Environmental Protection Agency and United States Environmental Protection Agency-recommended database were referred (US EPA, 2009; Mustafa et al., 2017; Nie et al., 2018). 3. Results and discussion 3.1. Volatile organic compound emissions from dustbins 3.1.1. Components and concentrations of volatile organic compounds The components and concentrations of VOCs detected in the community dustbins in different seasons are shown in Fig. 1. The values for mixed collection represent the VOC concentration in the mixed collection bins in the unclassified community, and the kitchen waste and other values indicate the concentration in the kitchen waste bins and other classified bins in the classified community, respectively. The previous studies have barely touched on the topic of VOC concentration in the dustbin, but were mainly focused on the concentration of VOCs in dustbins in different situations (Statheropoulos et al., 2005). Jiangsu Province is one of the largest regions contributing to VOC emissions in China (Zheng et al., 2016), and the release of VOCs cannot be ignored in residential communities. The types of VOCs detected in the community garbage bins mainly included aromatic compounds, sulfuric compounds, terpenes, alkanes, and halohydrocarbons. In terms of material composition, halohydrocarbons were the largest component and accounted for approximately 40%, followed by aromatic compounds (appx. 30%), and the percentage of sulfuric compounds was the lowest (appx. 5%) (Fig. 1). The total concentration of VOCs in mixed collection was the highest in summer (196.6 μg/m3), followed by that in autumn (121.8

100

0

MC

KW

O

MC

KW

O

MC

KW

O

MC

KW

O

Fig. 1. Seasonal changes in volatile organic compound concentrations emitted from dustbins. Abbreviations: MC, waste bins in mixed collection; KW, kitchen waste bins in classified collection; O, other waste bins in classified collection.

μg/m3), spring (94.4 μg/m3), and winter (48.2 μg/m3). In summer, owing to high temperature and humidity, microorganisms are active (Wu et al., 2010) and organic content, such as fruits and vegetables, is higher in the domestic waste. In addition, the high temperatures in summer promote the release of odorous gases in the dustbins (Capelli et al., 2008). Thus, the concentration of VOCs in summer in mixed collection was higher than in other seasons. However, the concentration of VOCs in kitchen waste and other waste dustbins was higher in spring and autumn and lower in summer and winter. From the viewpoint of domestic waste classification, the amount of VOCs detected in the dustbins was in this descending order: mixed collection, kitchen waste, and other waste. The concentration of VOCs was higher in kitchen waste than in other garbage because the moisture content and density of kitchen waste were high, and the easier formation of a local anaerobic zone caused the production of a large amount of VOCs (D'Imporzano et al., 2008). In conclusion, waste sorting will reduce the generation of VOCs at the source.

3.1.2. Terpenes There was a low production of terpenes in the domestic waste dustbins, and mainly included α-pinene, β-pinene, and limonene. The concentration of terpenes in the three dustbins types (household waste bins in mixed collection, kitchen waste bins in classified collection, and other waste bins in classified collection) for all seasons is shown in Fig. 2a. Among the types of terpenes present in each type of dustbin, the concentration of limonene was the highest, and particularly in winter, the proportion of limonene in mixed collection dustbins was 100%. Limonene is a characteristic degradation product of fresh MSW (Sadowska-Rociek et al., 2009). In summer, the concentrations of αpinene and β-pinene in mixed collection bins were higher than in other dustbins in other seasons owing to the complexity of garbage types and high temperatures. According to the seasons, the concentration of terpenes was higher in summer and autumn at 54.9 μg/m3 and 47 μg/m3, respectively, in kitchen waste dustbins. The highest terpene concentration observed in autumn might have been due to the high consumption of citrus fruits in autumn (Statheropoulos et al., 2005). In nature, terpenes mainly originate from plants (Griffin et al., 1999), such as from vegetable peels by oxidative decomposition (Wang et al., 1999; Wang and Wu, 2008; Moreno et al., 2014). Thus, the concentration of terpenes was the highest in kitchen waste bins, followed by that in mixed collection bins, and finally in other waste bins (appx. 10 μg/m3). Terpenes have a pleasant odor, but when mixed with other compounds, it becomes unpleasant. Thus, terpenes play an important role in waste odor perception (Müller et al., 2004; Statheropoulos

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40

Co n cen t r at io n ( μ g/m3)

Co n cen t rat i o n (μg / m3)

Undecane Dodecane Cyclohexane

α-pinene β-pinene Limonene

50

40

30

20

Decane

30

20

10 10

0

MC KW O Spring

MC KW O Summer

MC KW O Autumn

0

MC KW O Winter

MC KW O Spring

(a) 250

Ethanethiol Dimethyl sulfide Carbon disufifde Dimethyl disulfide

15

10

5

Ethylbenzene Chlorobenzene O-xylene Para-xylene Toluene P-cymene Styrene

200

Co n cen t rat i o n (μg ∙m3)

20

Co n cen t rat i o n (μg / m3)

MC KW O Winter

MC KW O Autumn

(b)

25

0

MC KW O Summer

Benzene 1,4-dichlorobenzene 1,3-dichlorobenzene 1,3,5-trimethylbenzene 1,2,4-trimethylbenzene 1,2,3-trimethylbenzene Benzylchloride

150

100

50

MC KW O Spring

MC KW O Summer

MC KW O Autumn

MC KW O Winter

0

MC KW O Spring

MC KW O Summer

MC KW O Autumn

MC KW O Winter

(d)

(c) 160

Chlorodibromomethane Methylbromide Tetrahydrofuran Carbontetrachloride Tribromoform Trichloroethylene Chloroform Chloroethane

140

Co n cen t rat i o n (μg / m3)

120 100

Trichlorofluoromethane Dichloromethane 1,2-dibromoethane 1,2-dichloroethane 1,2-dichloropropane Terachloroethylene Vinylidenechloride

80 60 40 20 0

MC KW O Spring

MC KW O Summer

MC KW O Autumn

MC KW O Winter

(e) Fig. 2. Concentrations of VOCs components emitted from dustbins. (a): terpene concentrations. (b): alkane concentrations. (c): sulfuric compound concentrations. (d): aromatic compound concentrations. (e): halohydrocarbon concentrations. Abbreviations: MC, waste bins in mixed collection; KW, kitchen waste bins in classified collection; O, other waste bins in classified collection.

et al., 2005). Considering the characteristics and concentration of terpenes, domestic waste should be classified. 3.1.3. Sulfur-containing compounds Sulfides are irritating and foul-smelling compounds that are emitted during garbage fermentation or food decay, and they have very low sensory thresholds (Landaud et al., 2008; Kim et al., 2009; Wu et al., 2010). High sulfide production was not observed, and mainly included ethanethiol, dimethyl sulfide (DMS), carbon disulphide (CS2), and dimethyl disulfide (DMDS) (Fig. 2c). Ethanethiol, a typical sulfur-

containing VOC, can emit a strong odor in the air at just a few ppb concentration (Kim et al., 2007). Ethanethiol was detected in the other waste dustbins only in summer, which mainly contained waste material. Few studies have shown that ethanethiol is detected in odorous substances (Son and Kim, 2015). DMS was detected only in kitchen waste and other waste bins in summer at concentrations of 3.9 μg/m3 and 0.3 μg/m3, respectively. In all seasons, DMDS was detected in dustbins, except in other waste dustbins in spring. In spring, DMDS was the only detected sulfur-containing compound, and in summer, the concentration of DMDS was the highest in mixed collection dustbins (16.6 μg/

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Table 2 Ozone formation potential of VOCs emitted from mixed collection and classified collection dustbins (μg/m3). VOCs

Terpenes Sulfuric compounds Benzenes Alkanes Total

Spring

Summer

Autumn

Winter

MC

KW

O

MC

KW

O

MC

KW

O

MC

KW

O

111.4 0.0 169.1 190.7 471.3

114.2 0.0 102.0 101.8 317.9

48.9 0.0 102.8 62.2 213.9

179.9 1.1 702.7 137.5 1021.2

212.4 0.8 100.0 174.0 487.2

39.4 0.8 52.9 12.2 105.3

122.6 1.0 394.5 47.4 565.5

202.0 0.9 403.0 3.0 608.9

41.9 0.1 278.8 1.6 322.5

100.1 0.2 174.4 0.8 275.5

110.0 0.2 135.3 1.0 246.5

46.1 0.1 128.3 0.5 175.0

MC: waste bins in mixed collection; KW: kitchen waste bins in classified collection; O: other waste bins in classified collection.

m3). CS2 was also detected, with the highest concentrations in summer with 4.5 μg/m3 in mixed collection bins, 3.9 μg/m3 in kitchen waste bins, and 3.2 μg/m3 in other waste bins. In addition, in winter, the concentrations of CS2 were the lowest at 0.9 μg/m3, 1.0 μg/m3, and 0.5 μg/m3, respectively. Statheropoulos et al. (2005) found that DMDS was the only detected VSC in a study on the concentration of VOCs in garbage bins. DMDS and DMS are the main VSC components in sludge and pig manure composting processes (Maulini-Duran et al., 2013; Zang et al., 2016). However, Zhang et al. (2016) observed that H2S was the main VSC component in the composting process of kitchen waste, and accounted for 85–94.21% of the total VSC emissions. In addition, studies have shown that methyl mercaptan is the main VSC in the composting process of MSW (Zhang et al., 2011). These studies showed that the components of VSCs are different according to different waste compositions. However, regardless of the components, the VSC will have a bad odor. There were clear seasonal differences in VSC composition, with a complex composition in summer while simple in spring and winter. In addition, the concentrations in summer and autumn were higher than in other seasons. The concentrations of VSCs in mixed collection dustbins were 12.6 μg/m3, 21 μg/m3, 18.7 μg/m3, and 7.7 μg/m3 in each season, respectively. The observed seasonal variation in VSC concentrations was consistent with that of a previous study (Han et al., 2018). The concentration of VSCs was highest in the mixed collection bins, and was more than two times than that in the classified collection bins. In summer, owing to the complexity of waste types and high temperatures, the concentration of VSCs was higher, but it reduced after classification. 3.1.4. Aromatic compounds Aromatic compounds are the main components of VOCs, and are neurotoxic, carcinogenic, and teratogenic. Aromatic compounds have also been considered the main precursors of secondary aerosols in the troposphere. A total of 14 aromatic compounds were detected in the dustbins in this study, and their composition varied significantly in each season (Fig. 2d). In summer, the concentration of aromatic compounds in the mixed collection bins was the highest at 204.6 μg/m3, of which p-xylene had the highest concentration (90.4 μg/m3), followed by o-xylene (39.9 μg/m3), and ethylbenzene (28.0 μg/m3). However, after classification, the concentration decreased rapidly. The concentration of aromatic compounds in other waste bins was the lowest. The main sources of aromatic compounds are camphor pills, insecticides, fungicides, spices, deodorants, paint inks, and plastics (Chen et al., 2010). In summer, the abuse of pesticides, fungicides, and plastics and the high temperatures may be the main reasons for the high concentration of aromatic compounds. Nevertheless, the situation in spring, autumn, and winter was completely different from that in summer. There was little difference in the concentration of aromatic compounds between spring, autumn, and winter, but the composition was different. In spring, the concentration of toluene was the highest, and accounted for approximately 30% of the total aromatic compounds, followed by ethylbenzene, which accounted for approximately 20%, and p-xylene, which accounted for approximately 10%. In autumn and winter, the concentration of toluene was the highest, followed by that of mxylene and ethylbenzene, which was consistent with the detection of toluene, ethylbenzene, and naphthalene by Statheropoulos et al.

(2005). However, the current study, naphthalene was not detected in the aromatic compounds. A large number of studies have shown that toluene is also the largest contributor to the concentration of aromatic compounds in landfills, composting plants, and other areas (Fang et al., 2012; Liu et al., 2016; Garg and Gupta, 2019). These seasonal and compositional differences may be due to the different types of wastes and environmental factors (Na and Kim, 2001; Zou et al., 2003) in each season. Although the emission of aromatic compounds after classification did not decrease significantly, the concentration of aromatic compounds decreased in some seasons. The clearest decline was in summer.

3.1.5. Alkanes The VOCs in the waste bins included four types of alkanes, namely undecane, dodecane, cyclohexane, and decane (Fig. 2b). These saturated alkanes mainly originate from waste paper, yard garbage, and food waste such as by the thermal degradation of soybean oil in cooking processes (Zhang et al., 2012; Wang et al., 2018a, 2018b). Alkanes accounted for a small proportion of the VOCs and Tan et al. (2017) also found similar results. The types of alkanes detected were different in different seasons, for instance, undecane and dodecane in spring, dodecane and decane in summer, cyclohexane and undecane in autumn, and cyclohexane in winter. The seasonal difference may be attributed to the different types of garbage (Duan et al., 2014). Besides the composition, the concentration also showed seasonal differences. The concentration of alkanes in spring and summer was higher than that in autumn and winter; e.g., the concentration in mixed collection bins was 38.4 μg/m3 in summer and only 0.7 μg/m3 in winter. The alkane concentration can be effectively reduced by classified collection. For example, in summer the concentration of alkanes in mixed collection bins was much higher than that in the classified collection bins, which was also observed in autumn.







Alkanes Bezenes Sulfuric Compounds Terpenes





 MC KW O Spring

MC KW O Summer

MC KW O Autumn

MC KW O Winter

Fig. 3. OFP percentages of VOCs emitted from mixed and classified collections. Abbreviations: MC, waste bins in mixed collection; KW, kitchen waste bins in classified collection; O, other waste bins in classified collection.

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Table 3 Carcinogenic risk calculation results. VOCs

Spring MC

5.65 × Ethylbenzene 10−6 7.64 × Styrene 10−7 7.69 × Benzene 10−7 4.58 × 1,4-dichlorobenzene 10−7

Summer MC

KW

O

MC

KW

O

MC

KW

O

4.79 × 10−6 4.50 × 10−7 4.44 × 10−7 7.87 × 10−7

5.31 × 10−6 4.68 × 10−7 3.60 × 10−7 9.41 × 10−7

1.20 × 10−5 3.56 × 10−6

1.48 × 10−6 8.54 × 10−7

7.79 × 10−7 1.11 × 10−6

0

0

0

0

0

0

1.73 × 10−10 1.52 × 10−10 8.00 × 10−10 2.63 × 10−11

1.67 × 10−10 2.09 × 10−10 1.14 × 10−9 3.66 × 10−11

8.01 × 10−11 8.91 × 10−11 5.84 × 10−10 1.55 × 10−11

6.53 × 10−11 3.25 × 10−11 1.07 × 10−9 1.11 × 10−11

7.01 × 10−11 2.20 × 10−11 6.06 × 10−10 7.90 × 10−12

6.86 × 10−11 1.88 × 10−11 5.76 × 10−10 7.98 × 10−12

4.78 × 10−6 7.71 × 10−7 1.22 × 10−7 2.67 × 10−7 2.91 × 10−6 1.09 × 10−8 8.19 × 10−6 9.13 × 10−8 3.27 × 10−5

3.76 × 10−8 5.23 × 10−8 4.13 × 10−8 9.25 × 10−8 7.48 × 10−7 4.08 × 10−9 1.38 × 10−6 1.73 × 10−8 4.71 × 10−6

2.68 × 10−6 1.23 × 10−7 3.01 × 10−8 1.03 × 10−7 4.77 × 10−7 2.86 × 10−9 3.26 × 10−6 1.42 × 10−8 8.59 × 10−6

0

0

0

0

0

0

2.42 × 10−11 6.29 × 10−11

1.64 × 10−11 1.05 × 10−10 1.71 × 10−9 6.31 × 10−10 3.56 × 10−13 8.01 × 10−11 1.31 × 10−11 4.11 × 10−9

1.86 × 10−13 4.37 × 10−11 4.29 × 10−12 1.38 × 10−9

8.88 × 10−12 6.38 × 10−11 6.62 × 10−10 3.65 × 10−10 2.81 × 10−13 6.79 × 10−11 1.08 × 10−11 2.36 × 10−9

1.01 × 10−11 6.11 × 10−11 4.12 × 10−10 3.61 × 10−10 1.74 × 10−13 4.94 × 10−11 9.25 × 10−12 1.61 × 10−9

7.89 × 10−12 5.35 × 10−11 4.01 × 10−10 3.63 × 10−10 1.74 × 10−13 5.10 × 10−11 8.04 × 10−12 1.56 × 10−9

O

MC

6.80 × 10−7 5.03 × 10−8

2.42 × 10−7 4.95 × 10−8

1.69 × 10−6 5.64 × 10−9 1.16 × 10−5 4.82 × 10−8 2.06 × 10−5

1.42 × 10−6 5.32 × 10−9 4.19 × 10−6 6.66 × 10−8 1.30 × 10−5

Trichloroethylene Trichloromethane Dichloromethane 1,2-dichloroethane 1,2-dichloropropane Total

1.04 × 10−6 7.29 × 10−9 5.85 × 10−6 4.28 × 10−8 1.50 × 10−5

Winter

O

Benzyl chloride 3.79 × Tetrachloroethylene 10−7 6.68 × Carbon tetrachloride 10−8

Autumn

KW

0 3.95 × 10−10 3.20 × 10−13 4.47 × 10−11 9.07 × 10−12 1.69 × 10−9

0 1.23 × 10−10 4.39 × 10−10 0

MC: waste bins in mixed collection; KW: kitchen waste bins in classified collection; O: other waste bins in classified collection.

Table 4 Non-carcinogenic risk calculation results. VOCs

Spring MC

Ethylbenzene O-xylene P-xylene Toluene Styrene Benzene 1,3,5-Trimethylbenzene 1,2,4-Trimethylbenzene 1,4-Dichlorobenzene Tetrachloroethylene Carbon tetrachloride Trichloroethylene Trichloromethane Dichloromethane 1,2-Dichloroethane 1,2-Dichloropropane 1,1-Dichloroethylene Total

4.87 × 10−4 1.19 × 10−3 1.79 × 10−3 1.73 × 10−4 9.66 × 10−5 9.20 × 10−3 7.63 × 10−3 9.60 × 10−3 1.46 × 10−4 6.52 × 10−4 8.51 × 10−3 2.29 × 10−2 1.29 × 10−3 3.40 × 10−3 2.59 × 10−4 1.15 × 10−2 8.87 × 10−4 7.98 × 10−2

Summer KW 4.13 × 10−4 9.69 × 10−4 3.05 × 10−4 1.36 × 10−4 5.68 × 10−5 5.31 × 10−3 5.83 × 10−3 5.14 × 10−3 2.51 × 10−4 1.17 × 10−3 6.40 × 10−3 2.16 × 10−2 2.10 × 10−3 2.63 × 10−3 5.16 × 10−4 1.30 × 10−2 2.88 × 10−4 6.61 × 10−2

O

MC 4.57 × 10−4 1.61 × 10−3 2.19 × 10−4 1.28 × 10−4 5.92 × 10−5 4.30 × 10−3 3.67 × 10−3 5.02 × 10−3 2.99 × 10−4 4.17 × 10−4 6.30 × 10−3 2.86 × 10−2 1.76 × 10−3 2.48 × 10−3 1.86 × 10−4 1.79 × 10−2 9.58 × 10−5 7.35 × 10−2

Spring KW

1.03 × 10−3 1.91 × 10−2 2.00 × 10−2 1.77 × 10−4 4.50 × 10−4

O

1.28 × 10−4 7.42 × 10−4 7.10 × 10−4

MC 6.71 × 10−5 0 3.96 × 10−4

0

0

1.08 × 10−4

1.41 × 10−4

0

0

0

3.28 × 10−2 2.90 × 10−2

3.82 × 10−3 6.16 × 10−3

4.33 × 10−3

0

0

0

0

1.33 × 10−3 1.56 × 10−2 1.87 × 10−1 3.62 × 10−3 5.07 × 10−3 3.63 × 10−4 2.46 × 10−2

9.00 × 10−5 5.25 × 10−3 6.47 × 10−2 9.30 × 10−4 1.90 × 10−3 6.12 × 10−5 4.67 × 10−3

2.12 × 10−4 3.84 × 10−3 7.19 × 10−2 5.92 × 10−4 1.33 × 10−3 1.45 × 10−4 3.84 × 10−3

3.40 × 10−1

8.93 × 10−2

8.68 × 10−2

Winter KW

4.04 × 10−4 5.35 × 10−3 3.11 × 10−3 1.41 × 10−4 3.42 × 10−4 5.99 × 10−3 4.89 × 10−2 3.81 × 10−2 1.39 × 10−4 2.35 × 10−4 3.34 × 10−3 0 1.00 × 10−3 1.87 × 10−3 1.00 × 10−4 2.04 × 10−3 1.24 × 10−3 1.12 × 10−1

3.89 × 10−4 3.68 × 10−3 2.66 × 10−3 2.54 × 10−4 4.69 × 10−4 8.57 × 10−3 3.75 × 10−2 2.92 × 10−2 1.95 × 10−4 1.60 × 10−4 5.58 × 10−3 4.99 × 10−2 1.60 × 10−3 2.08 × 10−3 1.80 × 10−4 2.95 × 10−3 1.06 × 10−4 1.45 × 10−1

1.87 × 10−4 2.17 × 10−3 1.28 × 10−3 2.41 × 10−4 2.00 × 10−4 4.37 × 10−3 4.76 × 10−2 1.29 × 10−2 8.24 × 10−5 0 6.54 × 10−3 1.28 × 10−2 0 1.09 × 10−3 9.81 × 10−5 9.63 × 10−4 2.13 × 10−4 9.08 × 10−2

1.53 × 10−4 1.26 × 10−3 1.32 × 10−3 1.37 × 10−4 7.30 × 10−5 8.01 × 10−3 5.96 × 10−3 1.32 × 10−2 5.90 × 10−5 8.64 × 10−5 3.39 × 10−3 1.93 × 10−2 9.26 × 10−4 1.64 × 10−3 1.53 × 10−4 2.43 × 10−3

5.82 × 10−2

KW 1.64 × 10−4 1.07 × 10−3 1.23 × 10−3 1.02 × 10−4 4.94 × 10−5 4.53 × 10−3 3.87 × 10−3 4.49 × 10−3 4.19 × 10−5 9.84 × 10−5 3.24 × 10−3 1.20 × 10−2 9.16 × 10−4 1.02 × 10−3 1.11 × 10−4 2.08 × 10−3 6.08 × 10−5 3.51 × 10−2

O 1.60 × 10−4 1.05 × 10−3 1.10 × 10−3 1.03 × 10−4 4.21 × 10−5 4.31 × 10−3 3.26 × 10−3 4.33 × 10−3 4.24 × 10−5 7.68 × 10−5 2.84 × 10−3 1.17 × 10−2 9.21 × 10−4 1.01 × 10−3 1.15 × 10−4 1.81 × 10−3

3.29 × 10−2

MC: waste bins in mixed collection; KW: kitchen waste bins in classified collection; O: other waste bins in classified collection.

Please cite this article as: X. Shi, G. Zheng, Z. Shao, et al., Effect of source-classified and mixed collection from residential household waste bins on the emissi..., Science of the Total Environment, https://doi.org/10.1016/j.scitotenv.2019.135478

X. Shi et al. / Science of the Total Environment xxx (xxxx) xxx

3.1.6. Halogenated compounds The concentration of halogenated compounds detected in dustbins was high, and accounted for approximately 40% of the total VOCs. The sources of halogenated compounds in domestic waste mainly comprised plastic, textiles, insulation foam and media in refrigeration and other equipment, and directly volatilized compounds in detergents (Scheutz et al., 2000; Statheropoulos et al., 2005). A total of 15 halogenated compounds were detected in the domestic waste bins, of which dichloromethane and 1,2-dichloroethane were found in higher concentrations (Fig. 2e). These results were consistent with those of Tan et al. (2017). However, in landfills, tetrachloroethylene had the highest concentration among halogenated compounds (Ding et al., 2012). The halogenated compound concentration was the highest in summer at 152.5 μg/m3 and the lowest in winter at 47.8 μg/m3. By classifying domestic waste, the concentration of halogenated compounds was reduced, especially in summer. The halogenated compound concentration in the kitchen waste bins and other waste bins was much lower than that in the mixed collection waste bins. 3.2. Ozone formation potential of volatile organic compounds VOCs are important precursors to the formation of ozone; thus, to evaluate the impact of VOCs on the atmosphere, the OFP of VOCs was examined. In this study, the MIR activity constant was used to calculate the OFPs of the different types of VOCs. Compared with other hydrocarbons, alkanes had fewer types and lower concentrations, so alkanes and halogenated hydrocarbons were classified into one class. In the followup study, all subsequent mentions of alkanes referred to the total amount of alkanes and halogenated hydrocarbons. The results are shown in Table 2. The contribution rate of the OFP varied with the volatilization concentration of different types of VOCs (Fig. 3). The contribution rate of VOCs to OFP varied for different dustbin types and seasons. The contribution rates of VOCs were in this descending order of magnitude: aromatic compounds, terpenes, alkanes, and sulfuric compounds. Especially in autumn and winter, the contribution to OFP was the highest. The reaction of aromatic compounds with hydroxyl radicals (OH•) or NOX contributed significantly to ozone formation, and the reaction products also contributed significantly to the formation of secondary organic aerosol (SOA) (Barthelmie and Pryor, 1997; Liu et al., 2016). Among all the VOCs, the OFP of sulfuric compounds was the lowest at less than 1 μg/m3, which can be neglected in total ozone formation. The total OFP of VOCs in different types of dustbins changed with the seasons (Supplementary Material Fig. S1). The total OFP of VOCs in the dustbins was of the same magnitude as that of coking plants and sewage treatment plants (Jia et al., 2009; Tang et al., 2011), but was lower than that of composting plants (Nie et al., 2019). Therefore, from the viewpoint of incremental reaction activity, residential domestic waste dustbins were a source of ozone in urban areas. The VOCs from mixed collection dustbins had the highest OFP, especially in summer, and reached 1.02 × 103 μg/m3. In autumn, the OFP of VOCs in kitchen waste dustbins was slightly higher than that in mixed collection dustbins, which might have been due to the higher concentration of aromatic compounds in kitchen dustbins in autumn. However, the OFP of VOCs in other waste bins collected after classification was much lower than that in mixed collection bins, and the OFP decreased by approximately 50%. Therefore, after classification, the OFP of VOCs decreased effectively, especially in summer. 3.3. Human health risk assessment The specific parameters of the evaluation method, including the CR levels, RFC, and IUR of related VOCs in domestic waste dustbins, are listed in the Supplementary Material (Table S1). According to the International Agency for Research on Cancer, the carcinogenicity of substances is divided into the following five grades:

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1, 2A, 2B, 3, and 4. The specific explanation is shown in the Supplementary Material (Table S2). CR is considered when its value is higher than 10−6 (US EPA, 2009), and can be divided into possible risks (lower than 10−5 and higher than 10−6), probable risks (lower than 10−4), and definite risks (higher than 10−4) (Durmusoglu et al., 2010; Li et al., 2013). The CR values of ethylbenzene, styrene, trichloromethane, and 1,2-dichloroethane in bins in summer were higher than 10−6, thus, CR was present (Table 3). Although there was no CR when the CR value of most VOCs was below 10−6, the accumulated CR value in the domestic waste bins indicated CR in spring and summer (probable risk in spring and possible risk in summer). The cumulative CR values of VOCs should be considered (Wu et al., 2018). Ethylbenzene and 1,2-dichloroethane were the main carcinogens in spring, and ethylbenzene in summer. Ethylbenzene is a harmful air pollutant that can cause a variety of health problems, such as cancer, respiratory irritation, and damage to the nervous system (US EPA, 2003). HR is considered to be present when its value is more than 1, and is considered negligible for a value less than 0.5. However, if the HR value is greater than 0.5 but less than 1, there is a health risk that needs to be paid close attention to (Durmusoglu et al., 2010; Nie et al., 2018). The HR values of the VOCs in dustbins are listed in Table 4. All values of HR were lower than 0.5, so there was no HR in the dustbins. 4. Conclusions Forty VOCs in total were observed in the domestic waste bins of residential communities. Among them, aromatic compounds contributed the most to the OFP. After classification, the concentration and OFP of VOCs were reduced. There was a CR in spring and summer, posing probable risks especially in the spring. The CR of VOCs in classified collection bins was lower than that of VOCs in mixed collection bins. Classified collection of domestic waste could decrease the generation and release of VOCs from the source, and could reduce the local atmospheric ozone generation and the consequent health risks to surrounding residents. Residents should be encouraged to classify waste in residential areas. In this study, Suzhou city in China was used as a case study to investigate the impact of the collection method on the total VOC emissions. In order to be more persuasive and typical, more sampling sites should be considered and analyzed via the regional differences. In addition, in order to further clarify the impact of the classified waste collection on the total VOCs, the impact mechanism needs to be analyzed in the future research works. Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper. Acknowledgments The work was supported by the National Natural Science Foundation of China (41371455) and the National Key Technology Research and Development Program of China (2014BAC02B01). Gratitude is extended to all for supporting our work during the study process. Appendix A. Supplementary data Supplementary data to this article can be found online at https://doi. org/10.1016/j.scitotenv.2019.135478. References Barthelmie, R.J., Pryor, S.C., 1997. Secondary organic aerosols: formation potential and ambient data. Sci. Total Environ. 205, 167–178.

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Please cite this article as: X. Shi, G. Zheng, Z. Shao, et al., Effect of source-classified and mixed collection from residential household waste bins on the emissi..., Science of the Total Environment, https://doi.org/10.1016/j.scitotenv.2019.135478