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Article

Toward more intercomparable road dust studies

Pages 826-855 | Published online: 13 Mar 2020

Abstract

Road dust (RDS) often contains elevated concentrations of pollutants, especially metals. Numerous studies were performed in the last two decades investigating the concentrations of metals like Cu, Pb, and Zn in RDS. In a literature search 177 studies were found where RDS bulk samples were analyzed. In another 49 studies the RDS samples were split into a number of size fractions to consider also the size dependence of the metal concentrations. In RDS bulk sample studies, the upper size limit (USL) of the RDS samples ranged from 2 µm to more than 2000 µm. This is partly a result of the different aims of the studies. However, the concentrations of metals in RDS particles are quite size-dependent. Consequently, comparing of results from different studies makes little sense. Based on the available literature, a standardized sample preparation sequence is proposed in this work. To serve the various aims of RDS studies the separation of the samples into four size fractions is suggested: <10 µm, 10–63 µm, 63–250 µm, and 250–2000 µm. The determination of the mass fractions of the size fractions parallel to the chemical analysis then allows calculation of the concentrations for RDS bulk samples with the four different USLs.

1. Introduction

In the last two decades, a large number of studies were carried out all over the world to determine the concentrations of metals in road dust or road-deposited sediments (RDS) with respect to the sources and transport pathways of the metals, their spatial distribution and their bio-availability and resulting risks to humans (Loganathan, Vigneswaran, & Kandasamy, Citation2013). Also the transformation processes in the RDS occurring in the environment were investigated (Jayarathne, Egodawatta, Ayoko, & Goonetilleke, Citation2019). A major source of metals like Cu, Pb, and Zn in the environment is road transport. The considerable technological improvements made in recent years helped to reduce the particulate matter emissions from combustion engine exhausts. Thus, the nonexhaust emissions of road transport such as those from RDS resuspension, brake wear, tyre wear, and road wear contribute to the ambient air particulate matter concentrations in cities to a similar extent than the tailpipe exhaust emissions (Amato et al., Citation2014), and RDS resuspension seems to be dominant in terms of particulate mass. This has increased the environmental concern related to RDS.

In the literature search covering the last 20 years, a total of 177 studies published in English were found reporting the concentration data of bulk RDS samples for metals like Cu, Pb, and Zn. Another 14 papers found were based on the same RDS concentration data as published in one of the studies. Studies investigating roadside topsoils where the upper few centimeters of the roadside soil were sampled were not included. A further 49 studies reported concentrations of metals for size-fractionated RDS samples. Close to half of these studiers (21 papers) also reported metal concentration data for the bulk RDS samples. In another 8 papers data of concentrations by particle size from previous studies were used.

The concentration of metals in RDS depends also on the size of the particles. Typically, the highest metal concentrations are found in the finest size fractions of the RDS. In a study by Al-Rajhi, Al-Shayeb, Seaward, and Eswareds (Citation1996), where the RDS samples were sieved into eight size fractions between 1.0–2.0 mm and <40 µm the maximum concentrations were two to six times the minimum concentrations depending on the metal. In a recent study the significant influence of the upper size limit (USL) for bulk RDS samples applied in the sample collection and preparation procedure on the concentration results was demonstrated (Lanzerstorfer & Logiewa, Citation2019). Depending on the metal the concentration of an RDS semple with an USL of 37 µm was found to be up to eight times higher compared to the same RDS sample with an USL of 2000 µm.

In many RDS studies, tables are presented comparing the concentration results with data from other studies. Thereby, results for RDS samples with quite different USLs—sometimes from 2 µm to 2000 µm—are often shown in the same table. In most of such tables the USL of the RDS samples is not even presented. Thus, comparison of the results makes little sense.

The aim of this work is to evaluate the RDS studies performed in the last two decades in order to gain a better understanding of the effect of the size dependence of the metal concentrations and to come up with feasible suggestions for future RDS studies which allow comparison of the results. gives an overview of the studies included in the evaluation.

Figure 1. RDS studies included in the evaluation.

Figure 1. RDS studies included in the evaluation.

2. Overview RDS studies

In this evaluation, 177 studies performed in the last two decades investigating the metal content of RDS bulk samples and 49 studies investigationg size-fractionated RDS samples were included. shows the number of studies performed each year. The year refers to the end of the RDS sampling period. If the sampling period was not reported in the study the date of submission for publication was used. Therefore, the numbers are quite low for the last few years. However, it can be assumed that some studies with samples collected in these years are ongoing or in submission status since in the evaluated studies the average time period between RDS sampling and publication was approximately 3 years.

Figure 2. Annual number of studies investigating RDS metal concentrations.

Figure 2. Annual number of studies investigating RDS metal concentrations.

The majority of the RDS bulk sample investigations were performed in Asia (67%), especially in China (36%). In contrast, studies investigating size-fractionated RDS were performed mainly in Europe (29%) and in China (27%).

In the literature two main methods are described for collecting RDS samples: on the one hand sweeping with a brush or a broom and collecting the sample with a dust pan and on the other hand vacuuming the road surface. Vacuum sampling is applied in different ways. For sampling of RDS from small areas dry or wet vacuum cleaners are used, while the discharge from street-sweeping vehicles gives an average sample for a large area. In approximately 90% of the studies the RDS sample collection method was descibed. In the RDS bulk studies the brush and dust pan method was mostly used (88%), while small-scale vacuum sampling was used in 9% and samples collected by street-sweeping vehicles were used in 3%. For the studies with sice-fractionated RDS samples the distribution of the used sampling methods was quite different: 53% small-scale vacuum sampling, 40% brush and dust pan sampling, and 7% samples from street-sweeping vehicles.

3. RDS bulk samples

Despite the importance of the USL, 22 out of 177 RDS bulk sample studies did not report a defined USL of the RDS samples. Some of these studies reported the manual removal of stones and other coarse debris. In the remaining 155 studies the USL applied was between 2 µm and 2000 µm. shows the frequency of USL use. The most frequently used USL was 2000 µm followed by 1000 µm and 63 µm. In most cases the USL was ensured by sieving with a mesh with the respective size. Only for achieving a USL of 10 µm or less the collected RDS samples were redespersed into air and then collected with a PM10 or PM2.5 sampling device. In one study the RDS was suspended in a sedimentation device and collected with a pipette (Nazzal, Rosen, & Al-Rawabdeh, Citation2013). On average, a slight trend to lower values of the USL can be observed over the years.

Figure 3. Frequency of use of various upper size limits (USLs) for RDS bulk samples.

Figure 3. Frequency of use of various upper size limits (USLs) for RDS bulk samples.

Most of the USLs used for RDS samples represent an upper limit of a soil size class according to Folk (Citation1974): 1000–2000 μm (very coarse sand), 500–1000 μm (coarse sand), 250–500 μm (medium sand), 125–250 μm (fine sand), 63–125 μm (very fine sand), 54–63 μm (silt and clay), and <54 μm (clay).

In several studies the USL chosen resulted from the aim of the study. In studies investigating the relation between air quality and RDS a USL of 10 µm (PM10) was usualy chosen (Amato et al., Citation2009; Chow, Watson, Ashbaugh, & Magliano, Citation2003; Kong et al., Citation2011). In many other studies the selected USL was also decided by the aim of the study. However, the choice of the USL is not always reasonable. The majority of the studies reported metal pollution in more general terms. The applied USL ranged from 2 µm (Nazzal et al., Citation2013) to 2000 µm. In several of the studies the spatial distribution of metals in an larger area was invetigated, Quite different USLs were applied, for example 2000 µm, 500 µm, and 125 µm (Ordonez, Loredo, DeMiguel, & Charlesworth, Citation2003; Shi et al., Citation2008; Tang, Ma, Zhang, & Mao, Citation2013). Also in studies dealing with the seasonal variation of metal concentrations in RDS, various values for the USL were used, ranging from 150 µm (Lin, Gui, Wang, & Peng, Citation2017) to 1000 µm (Robertson & Taylor, Citation2007).

Many studies dealt with the assesment of human health risk by RDS. The typical USL used in these studies was 63 µm (Hu et al., Citation2011; Li, Qian, Hu, Wang, & Gao, Citation2013; Saeedi, Li, & Salmanzadeh, Citation2012). However, USLs of 100 µm (Ferreira-Baptista & de Miguel, Citation2005), 125 µm (Shi et al., Citation2010), 850 µm (Ma & Singhirunnusorn, Citation2012), 1000 µm (Wang, Lu, Ren, Li, & Chen, Citation2014), and even 2000 mm (Kamani et al., Citation2017) were also used.

In studies investigating the relation between metal concentrations in RDS and stormwater runoff, USLs from 75 µm (Aryal et al., Citation2017) to 2000 µm (Brown & Peake, Citation2006) were used. Also in studies on source appointment quite different USLs, for example 37 µm, 125 µm, and 1000 µm (Pan, Lu, & Lei, Citation2017; Valotto et al., Citation2015; Žibret, Van Tonder, & Žibret, Citation2013) were applied. The same was found in studies comparing the metal concentrations in indoor and outdoor dust. The USLs ranged from 125 µm (Žibret & Rokavec, Citation2010) to 595 µm (Yaghi and Abdul-Wahab, Citation2004).

summarizes concentration results for Cu, Pb, and Zn from the 155 RDS bulk studies reporting a USL and the 21 studies with size-fractionated RDS reporting also results for the bulk RDS samples, which represent more than 9000 individual RDS samples. For each study the calculated average concentrations for all RDS samples were used. shows the concentrations of Cu, Pb, and Zn as a function of the USL applied in sample preparation. Especially for Cu and Zn the measured concentrations tend to be lower for larger values of the USL.

Figure 4. Concentrations of Cu, Pb and Zn as a function of the USL applied in sample preparation.

Figure 4. Concentrations of Cu, Pb and Zn as a function of the USL applied in sample preparation.

Table 1. Average RDS bulk sample concentrations of metals in 176 studies reporting the USL of the sample.

4. Size fractionated RDS samples

In 49 studies the metal concentration of RDS was reported for at least two different size fractions. The maximum number of size fractions was 11 and the average number was 4.9 ± 2.0. shows the size ranges of the RDS size fractions investigated in the various studies. An x-symbol at the upper limit of the largest size fraction indicates an estimate because in the study only the lower limit of the largest size fraction was reported. A wide variation of size limits for the various size fractions ranging from 1 µm to 3000 µm was found.

Figure 5. Size ranges of the RDS size fractions investigated.

Figure 5. Size ranges of the RDS size fractions investigated.

Size fractionation was performed in most cases by sieving, using meshes with the respective sizes. In some studies RDS samples were redespersed into air and the dust was collected, for example with a PM10, PM2.5, or PM1 sampling device (Chen, Wang, Liu, & Ren, Citation2012; Kong et al., Citation2012; Wang, Chang, Tsai, & Chiang, Citation2005) for achieving a separation at very small paricler sizes. In a few other studies air classification was applied (Lanzerstorfer, Citation2018; Lanzerstorfer & Logiewa, Citation2019; Logiewa, Miazgowicz, Krennhuber, & Lanzerstorfer, Citation2020) and in one study the RDS was suspended in a liquid for size fractionation (Padoan, Romè, & Ajmone-Marsan, Citation2017).

The reported concentrations are always for the size ranges between the limits except for the studies by Chen et al. (Citation2012) and by Kong et al. (Citation2012), where the data are for the whole size range from zero up to the maximum size.

In 30 studies the metal concentration data were presented in tables, while in 19 studies the data were shown in diagrams only. In both groups, the metal concentrations were higher in the finer size fractions of the RDS. However, investigation of the size dependence of the concentrations only the data from the tables could be used. The geometric mean of the size limits was used as a representative particle size for each size fraction except for the finest size fraction with the lower limit of zero, where the arithmetic mean was used. For each study the average concentrations for each size fractions were calculated. Generally, the concentrations are higher in the finer size fractions. However, the gradient of this trend is different in the various studies. The Cu concentration frequently shows deviations from the general trend of the size-dependence. Especially in the coarser size fractions >100 µm higher concentrations can be found. Such fluctuations are less frequently found for Pb and Zn. The gradients of the size dependence have a significantly higher negative value in comparison to the gradients in . This is because the data in show the average concentration for the dust samples from zero up to the applied USL.

To make results of the various studies comparable, relative concentrations were calculated, where the concentration was related to the concentration for a particle size of 63 µm. The theoretical concentration for a particle size of 63 µm was obtained by linear interpolation in a double-logarithmic scale using the nearest two data points. shows the results for Cu, Pb, and Zn. The exponent b of the regression function ci=Ai/xbi is a measure for the size dependence of the concentration. It was highest for Zn (0.38), followed by Pb (0.34), and was lowest for Cu (0.29). The highest correlation coefficient r2 was found for Zn (0.76), followed by Pb (0.65). The low correlation coefficient of 0.48 for Cu reflects the more frequent fluctuations of the Cu concentration as can be seen in .

Figure 6. Relative concentration of Cu, Pb, and Zn based on the calculated concentrations for a particle size of 63 µm.

Figure 6. Relative concentration of Cu, Pb, and Zn based on the calculated concentrations for a particle size of 63 µm.

5. Toward a standard for size limits in RDS sample preparation

In the comparison of RDS metal concentrations measured at different locations, results from studies were frequently used where different USLs were applied during sample preparation typically ranging from 63 µm to 2000 µm (Ferreira-Baptista & de Miguel, Citation2005; Manasreh, Citation2010; Saeedi et al., Citation2012). In several cases the values of USLs are even not shown in the tables (Christoforidis & Stamatis, Citation2009; Joshi, Vijayaraghavan, & Balasubramanian, Citation2009; Yu, Wang, & Zhou, Citation2014). In fact, in some studies average concentrations were calculated for samples with different USLs, for example USLs ranging from 125 µm to 2000 µm (Wei & Yang, Citation2010) or even from 10 µm to 2000 µm (Okorie, Entwistle, & Dean, Citation2012; Zafra-Mejía, Gutiérrez-Malaxechebarria, & Hernández-Peña, Citation2019).

However, the comparison of data of RDS samples or the calculation of an average from RDS samples with a different USL are quite meaningless. To make such investigations reliable a more standardized sample preparation would be useful. The following items have to be considered:

  • The produced data should be usable for assessments of various kinde (resuspension into the atmosphere, stormwater runoff, hazards, and risk)

  • The laboratory work should remain limited.

  • For sieving, similar mesh sizes according to US and ISO standards should be available

Because of the different requirements with respect to particle size resulting from the various aims of RDS studies the application of size fractionation of the RDS samples would be preferable instead of the investigation of RDS bulk samples only. Minimizing the number of size fractions produced for chemical analysis is recommended because of the related costs. The suggested limits for the RDS size fractions are summarized in .

Table 2. Suggested size fractions for RDS studies.

The most reasonable USL for the whole RDS sample and therefore for the largest size fraction is 2000 µm because this would be in accordance with the USL used in many RDS studies performed in the past.

In air quality studies PM10 is widely used (Amato et al., Citation2009; Chow et al., Citation2003; Kong et al., Citation2011). Therefore, 10 µm would be the most feasible upper limit for the finest size fraction. Additionally, experiments by Kuhns et al. (Citation2001) and Hussein, Johansson, Karlsson, and Hansson (Citation2008), where the increase of the airborne dust concentration behind the wheels of a driving car was measured for various size fractions, showed that resuspension of dust from the road surface into the air is mainly limited to particle sizes <10 µm. Therefore, this size fraction is representative for dust resuspension.

The mobility of RDS particles with stormwater runoff also strongly depends on the particle size. In a study by Kim and Sansalone (Citation2008) 65–99% of the particles in the effluent after the local particle separator were <75 µm. Therefore, studies investigating stormwater runoff usually concentrate on fine size fractions like <38 µm (Kayhanian, McKenzie, Leatherbarrow, & Young, Citation2012), <63 µm (Camponelli, Lev, Snodgrass, Landa, & Casey, Citation2010), or <75 µm (Li & Zuo, Citation2013; Liu, Liu, Li, & Guan, Citation2015). Particle size distribution measurements of the suspended solids in stormwater runoff showed that the particles are smaller than approximately 250 µm (Aryal et al., Citation2017). Thus, two further size fractions would be recommended: firstly 10–63 µm and secondly 63–250 µm. The 63 µm limit would serve for runoff studies and is also the USL of many road dust studies performed in the past. The 250 µm limit also fits well into the sequence since the representative particle size of the four size fractions are nearly equidistant on the logarithmic size scale.

With the exception of the separation of the finest size fraction <10 µm the proposed size limits were already used in a RDS study by Khanal, Furumai, and Nakajima (Citation2014). Additionally, the proposed size limits 63 µm, 250 µm, and 2000 µm were frequently used in studies with size fractionation of RDS samples ().

In a study the mass fractions of the four resulting size fractions 0–10 µm, 10–63 µm, 63–250 µm, and 250–2000 µm also have to be determined. Then the mass concentration of a component n can be calculated for the RDS samples for all three USLs. For the USL xk the concentration can be calculated from the concentrations in the size fractions smaller than this USL and the corresponding mass fractions of these size fractions using the following equation: cn(xxk)=i=1kcn,ixm,ii=1kxm,i. cn,i is the mass concentration of the component in the size fraction i and xm,i is the mass fraction of size fraction i.

If there would be a limitation in a study to have only one size fraction of RDS to be analyzed, maybe, it would be best to use an USL of 63 µm. On the one hand, this USL covers the requirements of stormwater runoff studies and on the other hand, it is the USL in the fine particle size range which has been used most frequently in the past. However, separating the RDS into the four size fractions mentioned above would always be preferable.

6. Conclusion

Because of concerns about metal pollution, RDS studies were performed all over the world. In most of the studies only RDS bulk samples were analyzed, while in some of the studies the RDS samples were split into a number of size fractions. As shown in many studies, the metal concentrations are substantially higher in the finest size fractions and lower in the coarse size fractions. As a result, the concentrations measured for RDS bulk samples depend on the USL applied during sample preparation. The USLs used in various studies range from 2 µm to 2000 µm. This is partly a result of the different aims of the studies, for example the influence of RDS resuspension on air quality or the transport of RDS with stormwater runoff. Under these circumstances, the comparison of results from different studies is quite limited. Therefore, a standardized sample preparation procedure is proposed. To serve the various aims of RDS studies separation of the RDS samples into four size fractions would be required: <10 µm, 10–63 µm, 63–250 µm, and 250–2000 µm. The chemical analysis of the size fractions together with the determination of the mass fractions allows the calculation of the concentrations for RDS bulk samples with the different USLs.

Acknowledgment

Proofreading by P. Orgill is gratefully acknowledged.

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