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Emitted from Residential Coal Combustion in High Lung Cancer Incidence Areas of China

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Emitted from Residential Coal Combustion in High Lung Cancer Incidence Areas of China processes Article Approval Research for Carcinogen Humic-Like Substances (HULIS) Emitted from Residential Coal Combustion in High Lung Cancer Incidence Areas of China Kai Xiao 1, Qingyue Wang 1,*, Yichun Lin 1, Weiqian Wang 1 , Senlin Lu 2,* and Shinich Yonemochi 3 1 Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura-ku, Saitama 338-8570, Japan; [email protected] (K.X.); [email protected] (Y.L.); [email protected] (W.W.) 2 School of Environmental and Chemical Engineering, Shanghai University, 99 Shangdalu, Baoshan District, Shanghai 200444, China 3 Center for Environmental Science in Saitama, 914 Kamitanadare, Kazo 347-0115, Japan; [email protected] * Correspondence: [email protected] (Q.W.); [email protected] (S.L.) Abstract: The incidence and mortality rate of lung cancer is the highest in Xuanwei County, Yunnan Province, China. The mechanisms of the high lung incidence remain unclear, necessitating further study. However, the particle size distribution characteristics of HULIS emitted from residential coal combustion (RCC) have not been studied in Xuanwei. In this study, six kinds of residential coal were collected. Size-resolved particles emitted from the coal were sampled by using a burning system, which was simulated according to RCC made in our laboratory. Organic carbon (OC), elemental carbon (EC), water-soluble inorganic ion, water-soluble potentially toxic metals (WSPTMs), water- Citation: Xiao, K.; Wang, Q.; Lin, Y.; soluble organic carbon (WSOC), and HULIS-C (referred to as HULIS containing carbon contents) in Wang, W.; Lu, S.; Yonemochi, S. the different size-segregated particulate matter (PM) samples were determined for health risk assess- Approval Research for Carcinogen Humic-Like Substances (HULIS) ments by inhalation of PM. In our study, the ratio of HULIS-Cx to WSOCx values in RCC particles Emitted from Residential Coal were 32.73–63.76% (average 53.85 ± 12.12%) for PM2.0 and 33.91–82.67% (average 57.06 ± 17.32%) Combustion in High Lung Cancer for PM2.0~7.0, respectively. The carcinogenic risks of WSPTMs for both children and adults exceeded −6 Incidence Areas of China. Processes the acceptable level (1 × 10 , indicating that we should pay more attention to these WSPTMs). 2021, 9, 1254. https://doi.org/ Exploring the HULIS content and particle size distribution of the particulate matter produced by 10.3390/pr9071254 household coal combustion provides a new perspective and evidence for revealing the high incidence of lung cancer in Xuanwei, China. Academic Editor: Adam Smoli´nski Keywords: residential coal combustion; HULIS-C; WSOC; carcinogenic risks; Xuanwei Received: 26 June 2021 Accepted: 19 July 2021 Published: 20 July 2021 1. Introduction Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in Atmospheric particulate matter has received more attention as air pollution has caused published maps and institutional affil- about seven million premature deaths every year. Fine particles (PM2.0 or smaller) are iations. generally more dangerous and ultrafine particles (one micron in diameter or less), which can penetrate tissues and organs, pose a greater risk of stroke, heart disease, chronic obstructive pulmonary disease, lung cancer and acute respiratory (https://www.who.int/; accessed on 18 May 2021). Solid fuels are still the main energy source for cooking and heating in some rural areas of China. In 2019, about 2.7 billion tons of coal were consumed in China, Copyright: © 2021 by the authors. Licensee MDPI, Basel, Switzerland. which contributed about 68.6% of the national primary energy source (http://www.stats. This article is an open access article gov.cn/tjsj/ndsj/; accessed on 18 May 2021). RCC are important anthropogenic sources distributed under the terms and of particulate and toxic and hazardous pollutants in the atmosphere [1]. The particles conditions of the Creative Commons generated from RCC produce reactive oxygen species (ROS), especially once it enters the Attribution (CC BY) license (https:// human body. Oxidative stress in the airways and alveoli leads to stimulation of alveolar creativecommons.org/licenses/by/ macrophages and injury to the epithelial lining, which in turn attracts inflammatory cells 4.0/). from the circulation [2]. This mechanism is considered to be related to highly redox-active Processes 2021, 9, 1254. https://doi.org/10.3390/pr9071254 https://www.mdpi.com/journal/processes Processes 2021, 9, x FOR PEER REVIEW 2 of 19 Processes 2021, 9, 1254 2 of 18 of alveolar macrophages and injury to the epithelial lining, which in turn attracts inflam- matory cells from the circulation [2]. This mechanism is considered to be related to highly redox-active components in the particulate matter. The identified amounts of metals and quinonescomponents are responsible in the particulate for only matter. a very Thesmal identifiedl mass concentration amounts of ofmetals particulate and matter quinones in theare atmosphere. responsible Recently, for only an avery abundant small water- masssoluble concentration organic ofcomponent, particulate namely matter HULIS, in the hasatmosphere. been identified Recently, as highly an abundant redox-active water-soluble and contributes organic to component, the oxidation namely potential HULIS, of particulatehas been identified matter [3,4]. as highly redox-active and contributes to the oxidation potential of particulateHumic-like matter substances [3,4]. are large molecules of unresolved water-soluble organic car- bon withHumic-like a polycyclic substances ring or are carboxyl, large molecules carbonyl, of unresolvedand hydroxyl water-soluble group structure organic [5], carbon con- sistingwith a of polycyclic 9–72% of ringWSOC or [6]. carboxyl, They have carbonyl, been widely and hydroxyl reported group in atmospheric structure [aerosols5], consist- in urbaning of [7], 9–72% rural, of forested WSOC [[8],6]. and They marine have beenenvironments widely reported [9], as well in atmosphericas rainwater aerosols[10], cloud in waterurban [11], [7], rural,and fog forested [12], with [8], andconcentrations marine environments varying over [9], two as well orders as rainwater of magnitude [10], cloudfrom water [11], and fog [12], with concentrations varying over two orders of magnitude from below 0.1 μg m−3 to dozens of μg m−3 [7]. HULIS was found to enhance catalytically the below 0.1 µg m−3 to dozens of µg m−3 [7]. HULIS was found to enhance catalytically generation of ROS under simulated physiological conditions, thereby likely may contrib- the generation of ROS under simulated physiological conditions, thereby likely may con- ute to PM-related health problems [13–15]. Many studies have shown that biomass com- tribute to PM-related health problems [13–15]. Many studies have shown that biomass bustion and secondary formation in the atmosphere are considered important sources of combustion and secondary formation in the atmosphere are considered important sources HULIS [8,16–18]. As for their health effects, redox sites on HULIS can promote electron of HULIS [8,16–18]. As for their health effects, redox sites on HULIS can promote electron transfer, leading to the production and conversion of excess ROS during respiratory dep- transfer, leading to the production and conversion of excess ROS during respiratory deposi- osition, thus disrupting the redox homeostasis of affected cells [3,17]. Subsequent intra- tion, thus disrupting the redox homeostasis of affected cells [3,17]. Subsequent intracellular cellular stimulation of oxidative stress may activate downstream pathways leading to var- stimulation of oxidative stress may activate downstream pathways leading to various ious respiratory and cardiovascular diseases [19]. It has recently been suggested that RCC respiratory and cardiovascular diseases [19]. It has recently been suggested that RCC is a issignificant a significant and and major major source source of HULISof HULIS [5], [5 which], which has has been been accepted accepted as as the the main main cause cause of ofhuman human lung lung cancer cancer [20 [20–23].–23]. XuanweiXuanwei has has the the highest highest incidence incidence and and mortality mortality rate rate of of lung lung cancer cancer in in China China [1]. [1]. AccordingAccording to to the the “2012 “2012 Chinese Chinese Cancer Cancer Regist Registryry Annual Annual Report,” Report,” the the average incidence raterate of of lung lung cancer inin XuanweiXuanwei waswas 92 92 per per 100,000, 100,000, which which is is four–five four–five times times higher higher than than the thenational national rate rate [24]. [24]. The incidenceThe incidence of lung of cancerlung cancer among among non-smokers non-smokers is 400/100,000 is 400/100,000 [25,26], [25,26],which iswhich 20 times is 20 highertimes higher than the than national the national average, average, especially especially among among women women in rural in ruralareas areas [20,27 [20,27,28].,28]. However, However, the particlethe particle size size distribution distribution characteristics characteristics of HULISof HULIS mitted mit- tedfrom from RCC RCC has has not not been been studied studied in Xuanwei. in Xuanwei. RuralRural houses houses in in the the Xuanwei Xuanwei area area are are mainly mainly two-story two-story civil civil structures structures (Figure (Figure 1a).1a). TheThe first first half half of of the the first first floor floor of of this this type type of of house house is isthe
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