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Characterization of Natural and Affected Environments

Characterization and risk assessment of atmospheric PM2.5 and PM10 particulate-bound PAHs and NPAHs in Rwanda, Central-East Africa Egide Kalisa, Edward Gou Nagato, Elias Bizuru, Kevin C Lee, Ning Tang, Stephen B Pointing, Kazuichi Hayakawa, Stephen Archer, and Donnabella C Lacap-Bugler Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.8b03219 • Publication Date (Web): 16 Oct 2018 Downloaded from http://pubs.acs.org on October 17, 2018

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Environmental Science & Technology

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Characterization and risk assessment of atmospheric

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PM2.5 and PM10 particulate-bound PAHs and NPAHs

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in Rwanda, Central-East Africa

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Egide Kalisa†∥, Edward Gou Nagato‡, Elias Bizuru∥, Kevin C Lee†, Ning Tang‡,

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Stephen B Pointing§, Kazuichi Hayakawa‡, Stephen DJ Archer†*, Donnabella C Lacap-

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Bugler†*

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† Institute for Applied Ecology New Zealand, School of Science, Auckland University of

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Technology, Auckland 1142, New Zealand

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‡ Institute of Natural and Environmental Technology, Kanazawa University, Kakuma-

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machi, Kanazawa, Ishikawa 920-1192, Japan

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§ Yale-NUS College and Department of Biological Sciences, National University of

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Singapore, Singapore 138527

1 ACS Paragon Plus Environment


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∥ School of Sciences, College of Science and Technology, University of Rwanda, P.O.

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Box 4285, Kigali, Rwanda

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ABSTRACT

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Exposure to airborne particulates is estimated as the biggest cause of premature human

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mortality worldwide and is of particular concern in sub-Saharan Africa where emissions

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are high and data is lacking. Particulate matter (PM) contains several toxic organic

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species including polycyclic aromatic hydrocarbons (PAHs) and nitrated PAHs (NPAHs).

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This study provides the first characterization and source identification for PM10 and PM2.5

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-bound PAH and NPAH in sub-Saharan Africa during a three-month period that spanned

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dry and wet seasons at three locations in Rwanda. The 24-hour mean PM2.5 and PM10

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concentrations were significantly higher in the dry than the wet season. PAH and NPAH

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concentrations at the urban roadside site were significantly higher than the urban

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background and rural site. Source identification using diagnostic ratio analysis and

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principal component analysis (PCA) revealed diesel and gasoline-powered vehicles at

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the urban location and wood burning at the rural location as the major sources of PAHs

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and NPAHs. These data demonstrate that PM concentrations and lifetime cancer risks

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resulting from inhalation exposure to PM-bound PAHs and NPAHs exceeded World



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Health Organization safe limits. This study provides clear evidence that an immediate

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development of emission control measures is required.


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INTRODUCTION

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Air pollution is the single largest cause of premature mortality worldwide with annual

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deaths estimated at seven million.1 Approximately 90% of these deaths are estimated to

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occur in low and middle-income countries, particularly sub-Saharan Africa.1 The World

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Health Organization (WHO) has air quality programs for most of the world's regions, some

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of which aim to assist countries in developing sustainable air quality policies. However,

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little data and no standards around air quality exist for sub-Saharan African countries

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such as Rwanda.2,3

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Rwanda is a landlocked country of 26,338 square kilometers and is the second most

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densely populated country in Africa with 12 million inhabitants. Despite undergoing a rapid

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urbanization,4 there is limited data on its ambient air quality and the identity of primary air

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pollution sources. The evaluation of particulate air pollution for a country is typically

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measured by the metrics of PM2.5 (particulate matter with aerodynamic diameter less than

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2.5 micrometres) that can enter the lungs and PM10 (particulate matter with aerodynamic

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diameter less than 10 micrometres) that are trapped in the nasopharyngeal tract causing



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adverse health impacts.5 To date, only a single research study on household PM2.5 was

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conducted in Rwanda, and this estimated that air pollution from cooking fuel combustion

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was the major risk factor for the countrywide burden of disease.6 No other air quality data

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(aside for satellite estimates) is available for the rest of the country.

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PM contains several toxic organic species including polycyclic aromatic hydrocarbons

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(PAHs) and nitrated PAHs (NPAHs), which are well known for their carcinogenic and

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mutagenic properties.7 Given their toxicity and their wide distribution, the United States

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Environmental Protection Agency (US EPA) has classified 16 PAHs priority compounds.8

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Their nitro derivatives, which exist at concentration orders of magnitude lower than PAHs,

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are nonetheless potentially more dangerous since they do not undergo an initial

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enzymatic activation process as for PAHs.7,9 PAHs and NPAHs are mainly released

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directly from anthropogenic activities and are products of incomplete combustion of

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organic materials such as coal, oil, petrol, and wood.10–13 Although NPAHs can be formed

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also as secondary compounds between atmospheric reaction of PAHs and atmospheric

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oxidants such as ozone and nitrate radicals,14 they are also suitable as tracers for the

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identification of ambient air pollution sources and photochemical pathways.15 Data on 6 ACS Paragon Plus Environment

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atmospheric PAHs and NPAHs is lacking for sub-Saharan Africa. Only two publications

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on NPAHs exist for the rest of Africa (Egypt and Algeria) and similar emissions scenarios

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suggest that NPAH are also likely a previously unmeasured risk in Rwanda.16,17

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In this study, we report atmospheric PM2.5 and PM10 and associated PAH and NPAH

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from three different usage areas in Rwanda during a three-month period in 2017. The

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objectives of this study were: (1) to investigate PAHs and NPAHs abundance and

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speciation in PM2.5 and PM10, (2) to identify their possible sources based on variation of

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spatial and temporal concentration, (3) to evaluate lifetime cancer risks resulting from

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inhalation exposure to PM-bound PAHs and NPAHs from urban and rural areas in

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Rwanda. This study provides the first empirical evidence for spatio-temporal trends in

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PM2.5 and PM10 -bound PAH and NPAH in sub-Saharan Africa and will serve as the basis

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for the development of standards by the Rwanda Environmental Management Authority

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(REMA) responsible for air quality monitoring and management.

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METHODS

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Sampling information

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PM2.5 and PM10 samples were collected daily at three locations in Rwanda (Figure 1).

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The urban background site was located away from emission sources such as industries

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and broadly representative of city-wide background conditions. The urban roadside site

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experiences high traffic volumes with frequent gridlock from mototaxis, buses, and

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personal vehicles. The rural area was situated approximately 100 km away from Kigali,

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was generally open with agricultural fields, minimal residential area, and distanced as far

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as possible from roads and industrial. Sampling sites were located on rooftops

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approximately 10~15 m above ground level. Two seasonal (wet and dry) sampling

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intervals were conducted at urban background and urban roadside. Sampling at the rural

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site was conducted during the wet season only. Details of the sampling sites

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characteristics were summarized in the Supporting Information (SI) (Table S1).

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Each sample was collected on a Whatman glass microfiber filter (GFF, Whatman EPM

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2000) using high-volume samplers (SIBATA Electric Company Limited, Japan, and HVS-


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RW-1000F) operated at 1000L/min for a period of 24 hours (from 12:00 am to 12:00 am

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of the following day). A total of 88 samples (PM2.5 and PM10) were collected from the three

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sites in 2017 and were analyzed for PAHs and NPAHs. Quality control (QC) and quality

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assurance (QA) detailing all information about filter handling, filter storage and gravimetric

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analysis were described in Text S1 of the SI. Meteorological data including temperature

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(T), relative humidity (RH), wind speed (WS) and wind direction (WD) for both urban and

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rural sites were obtained from synoptic weather stations of Rwanda meteorological

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weather stations situated close to the sampling sites.

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Figure 1. The sampling locations in Rwanda with reference to the African continent.

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Figure modified from yourfreetemplates.com. (Full details

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Extraction and Instrumental Analyses

here: https://yourfreetemplates.com/terms-of-use/)

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The extraction, instrumental analyses and standards used have been described in

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Hayakawa et al. (2018)18 and are detailed in Text S2 of the SI. Briefly, 15 individual PAHs

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(US EPA 610 PAH mixture of 16 PAHs except Acenaphthylene (Acyl) that does not

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fluoresce with the method used) and eight individual NPAHs (two NPAHs such as 2-

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nitropyrene (2-NP) and 2- nitrofluoranthene (2-NFR) were grouped together because they

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were not resolved completely). Therefore, 15 PAHs and 7 NPAHs were quantified in

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samples using two high-performance liquid chromatographic systems (HPLC-10A series,

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Shimadzu Inc., Kyoto, Japan), with one system equipped with a fluorescence detector

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and another equipped with a chemiluminescence detector.

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Data Analysis

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Principal component analysis (PCA) has been successfully applied in several aerosols

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studies to determine the source of PAHs and NPAHs based on spatial distribution of

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datasets.19–21 In this study, PCA using Statistical Analysis Software (SAS, version 9.4 by

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SAS institute Inc. Cary.INC. USA) was performed on all PAHs and NPAHs data as one

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unit. PCA results were presented by loading and score plots. PCA was used in

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conjunction with NPAHs to PAHs diagnostic ratio approaches to further understand the

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PAH and NPAHs concentrations in relation to their potential sources in the atmospheric

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environment of Rwanda. Three days back trajectories were calculated using the Hybrid

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Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model to determine the origin

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of air masses and establish source-receptor.22 As PAHs and NPAHs data were not

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normally distributed, a non-parametric test with SAS was used for analysis. Therefore,

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the Wilcoxon-Mann-Whitney test was used to compare two groups and a Kruskal-Wallis

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test was used to compare more than two groups.



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Environmental health risk assessment

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To evaluate cancer risk of PAHs and NPAHs detected in ambient air of Rwanda, we

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used a widely applied methodology developed by the US EPA.23,24 In the environment,

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PAHs are found as mixtures and benzo(a)pyrene (BaP) is used as PAH reference

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chemical due to its high carcinogenic potency and its well characterised toxicity.13 The

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carcinogenic risk was, therefore, estimated by using toxic equivalent factors (TEFs) for

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each PAH or NPAH compared to BaP.25 The concentration of each PAH or NPAH was

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converted to the BaP equivalent (BaPeq, carcinogenic equivalents, ng/m3) concentration

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by multiplying the concentration of PAHs with the corresponding TEF. TEF is the toxic

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equivalency factor of the compounds (PAHs and NPAHs). TEF values for 15 PAHs and

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2 NPAHs were obtained from the literature.23,26,27

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The excess cancer risk of people living in urban and rural areas in Rwanda was

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calculated based on EPA guidance for inhalation risk assessment following the

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equation.23

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Cancer risk (CR) = URBaP × BaPeq


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where URBaP is the inhalation cancer unit risk factor of BaP.

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The UR BaP (unit risk) is defined as the number of people at higher risk of cancer from

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inhalational exposure to 1 ng/m3 of a BaP equivalent concentration over a lifetime of 70

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years. The USEPA value of UR BaP is1.1 × 10–6 (ng/m3)–1 and estimates the lifetime

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cancer risks due to PAH and/or NPAH exposures.28

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RESULTS AND DISCUSSION

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Concentrations of PM2.5 and PM10

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The mean 24-hour concentrations of PM2.5 and PM10 were higher in urban sites (urban

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roadside: 185.3 µg/m3 and 214.0 µg/m3; and urban background: 81.4 µg/m3 and 98.7

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µg/m3), while the lowest concentrations were measured at the rural site (45.0 µg/m3 and

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53.7) for PM2.5 and for PM10, respectively. At the urban roadside, the 24-hour mean

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concentration of PM exceeded four times the WHO’s guideline for PM2.5 and for PM10 (25

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μg/m3, 50 μg/m3 respectively)29 (Table S2 of the SI). A Kruskal Wallis test showed that

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PM2.5 and PM10 median concentrations at the urban roadside site were significantly higher



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than urban background and rural sites (Table S3 of the SI). Wilcoxon-Mann-Whitney test

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showed that the median 24-hour PM2.5 and PM10 concentrations were significantly lower

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in the wet season than the dry season for both urban background and urban roadside

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sites (Table S4 of the SI). At the urban background site, a significant reduction of nearly

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55.4 % of median concentration of PM10 was measured between dry (146.3 µg/m3) and

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wet seasons (65.2 µg/m3) (p 0.5 have been reported to suggest combustion of wood and

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kerosene.49,50 This has also been reported in savanna fire particulate. Back trajectory

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analysis indicated that Rwanda’s air quality could experience increase PM from

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transported savanna and forest fire emissions from nearby East African countries (Figure

or

[Flu]/([Pyr]+[Flu])


ratio

>

0.5

and


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S1 of the SI). The [BaA]/([Chr]+[BaA]) ratio values of 0.38 - 0.64, >0.35 and 0.42 - 0.62

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have been proposed for diesel engine, gasoline engine and wood burning, respectively

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47,51,52.

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vehicle exhaust emissions (diesel & gasoline engine) and wood burning were the

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dominant sources of PAHs in urban and rural sites, respectively.

The values obtained between dry and wet season in the three sites, suggest that

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In addition to the primary combustion sources, NPAHs may also originate from

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atmospheric secondary formation.53 The concentration ratio of 2-nitrofluoranthene [2-

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NFR]/1-nitropyrene [1-NP] or [2-NFR]/[1-NP] has been used to investigate the relative

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contribution of NPAHs from primary formation vs secondary formation. A [2-NFR]/[1-NP]

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a value >5 indicates a strong contribution from secondary formation while value 5 was observed at all three sites (Table S11 of the SI) and was

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higher at urban background followed by rural area and urban roadside, providing further

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possible evidence for the contribution of NPAHs secondary formation. This indicates that

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there may be substantial secondary background formation in areas with lower volumes

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of road traffic, which is consistent with a previous study that indicated [2-NFR]/[1-NP]

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ratios are generally higher at suburban sites relative to their proximate urban site.58

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Source analysis of PAHs and NPAHs using PCA

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To further elucidate the potential sources of PAHs and NPAHs, PCA was used in

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conjunction with NPAHs to PAHs diagnostic ratio analysis (Figure 3). PCA results

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indicated that diesel and gasoline-powered vehicles at the urban locations and wood

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burning at the rural location were the major sources of PAHs and NPAHs and were

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consistent with diagnostic ratio source analysis. Detailed results and discussion on PCA

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source analysis are found in Text S4 of SI. In addition, PCA was performed on all PAH

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and NPAHs detected in both dry and wet season suggesting a seasonal effect on the



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concentrations, especially at the urban background with lower volumes of road traffic

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(Figure S6 of the SI).

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Figure 3. Multivariate analysis of particulates-bound polycyclic aromatic hydrocarbons

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(PAHs) and nitrated PAHs (NPAHs) at three sites in Rwanda. Principal component

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analysis (PCA) A) loading plots and B) score plots for the first two components of all PAHs

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and NPAH from three sites: (a) urban background (UB = blue), (b) rural (Rs = green) and (c) urban

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roadside (UR = red).

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Risk assessment

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The estimated cancer risks for the three sites were calculated from the concentrations

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of 15 PAHs and 2 most carcinogenic NPAHs (1-NP and 1.8-DNP). Total BaP equivalents

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(BaPeq) for the study period were highest in urban roadside followed by rural site and

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urban background (Table S12 of the SI). These results are comparable with other

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observations in Turkey (11 ng/m3) during non-heating periods59 but relatively higher than

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the values in western developed countries such as the United States (0.450 ng/m3)60 and

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Italy (0.79 ng/m3).61 There is a lower BaPeq carcinogenicity in western developed

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countries than that obtained in Rwanda, which can be attributed to rigorous emission

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standards, cleaner energy sources, more efficient industrial technology and lower

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population. Although the atmospheric concentrations of total NPAHs were lower than

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those of total PAH (Table S12 of the SI), and the risks were calculated using only two

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NPAHs. The total cancer risks calculated from 15 PAHs and 2 NPAHs was much higher

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at the urban roadside site than those in urban background and rural sites (Table S12 of

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the SI). These values obtained at each site exceeded the USEPA guideline (10−6),24 which

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suggests adverse health effects and would be classified as a definite risk (a carcinogenic

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risk greater than 1×10−4).62 Because abundant NPAHs such as 9-NA, 2-NP+2-NFR, were 31 ACS Paragon Plus Environment


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not determined and were excluded from the calculations due to the unavailability of TEF

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values, the values presented in this study are underestimated risks. Thus, toxicological

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of NPAHs data is urgently required to enable accurate risk assessments of atmospheric

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NPAHs. Overall, better monitoring of air quality as a mean to assess the risks of human

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exposure to PM -bound PAHs and NPAHs would enable the development of strategies

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to reduce the air pollution health burden, and facilitate urban planning. Future study

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should use other methods of source apportionment available for larger datasets such as

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positive matrix factorization.

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ASSOCIATED CONTENT

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Acknowledgements

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This research was supported by grant JSP-AUT1401-JR from the Royal Society of New

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Zealand. Financial support for the research was also provided by Yale-NUS College. We

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thank Kanazawa University for providing sampling equipment. S.D.J.A is grateful to

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Auckland University of Technology for a postdoctoral fellowship. E.K. is the recipient of a

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Commonwealth Scholarship for postgraduate study. K.H is grateful to JSPS Program for

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Advancing Strategic International Networks to Accelerate the Circulation of Talented 32 ACS Paragon Plus Environment

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Researchers (2015-2017). We also thank the Government of Rwanda, University of

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Rwanda, Rwanda Ministry of Environment and Rwanda Energy Group for providing

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permits, field and logistical support during the sampling campaign.

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Supporting Information

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Detailed information for extraction, standards and instrumental analyses, descriptive

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statistics, and results. Also included results on source analysis and carcinogenic risk. This

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material will be available free of charge via the internet at http://pubs.acs.org.

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AUTHOR INFORMATION

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Corresponding Authors

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*E-mail: [email protected]; [email protected]

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Notes: All authors declare no competing financial interest.

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