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原煤块和洁净煤燃烧产生的双亲代、含氧代和含硝代多环芳烃:排放因子、源特征及健康风险。

Parent, alkylated, oxygenated and nitro polycyclic aromatic hydrocarbons from raw coal chunks and clean coal combustion: Emission factors, source profiles, and health risks.

机构信息

Department of Environmental Science and Engineering, Xi'an Jiaotong University, Xi'an 710049, China; State Key laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710049, China.

Department of Environmental Science and Engineering, Xi'an Jiaotong University, Xi'an 710049, China; State Key laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710049, China.

出版信息

Sci Total Environ. 2020 Jun 15;721:137696. doi: 10.1016/j.scitotenv.2020.137696. Epub 2020 Mar 5.

Abstract

Residential coals are still inevitable using in developing areas in China. Clean coal briquettes, normally using alkaline substance such as lime or red mud (RM) as the additive, were helpful in pollution emission reduction even without changes of stoves. Studies of atmospheric polycyclic aromatic hydrocarbons (PAHs) emission characteristics from RM clear coal combustion were limited. In this study, emission factors (EFs), sources profiles, and health risks of polycyclic aromatic hydrocarbons (PAHs) in PM were investigated for raw coal chunks and clean coal (with red mud) through combustion experiments. EFs of total PAHs were found to be 160.1 ± 100.9 mg·kg and 19.4 ± 6.1 mg·kg for bituminous and anthracite raw coal chunks (B-C and A-C), respectively. EFs values were highest for parent PAHs (p-PAHs), followed by oxygenated PAHs (o-PAHs), alkylated PAHs (a-PAHs), and nitro PAHs (n-PAHs). EFs of p-PAHs account for 80% and 52% of total PAHs emissions for B-C and A-C, respectively, while those for o-PAHs are 22.9% and 44.9%, demonstrating residential coal combustion as a significant primary source for p-PAHs and o-PAHs. Clean coals were developed through cold-press technology with red mud (RM) as additive, and clean coals with RM contents of 10% are referred to as B-10% (bituminous) and A-10% (anthracite). Compared to raw coals chunks, EFs were reduced from 128.1, 2.5, 29.3 mg·kg and 161.8 μg·kg to 83.5, 1.3, 16.4 mg·kg and 102.2 μg·kg by B-10%, and from 10.1, 0.6, 8.7 mg·kg and 20.6 μg·kg to 11.9, 0.2, 2.4 mg·kg and 15.3 μg·kg by A-10% for p-PAHs, o-PAHs, a-PAHs and n-PAHs, respectively. Diagnostic ratios of 5-Nitroacenaphthene / Acenaphthene (0.02-0.05 for coal, 0.0002 for biomass) can be used to separate residential coal and biomass burning in source analysis. When B-C was replaced by B-10%, both noncancer (0.58 to 0.33 for male, 1.65 to 0.95 for female in hazard quotient) and cancer risks (5.68 × 10 to 2.73 × 10 for male, 2.63 × 10 to 1.27 × 10 for female) can be reduced. o-PAHs should be paid more attention because of its high cancer risks caused by 6H-Benzo(C,D)Pyrene-6-One (1.74 × 10 for male, 8.07 × 10 for female), which are even more than the total risks caused by n-PAHs (3.59 × 10 for male, 1.66 × 10 for female). Results from this study highlighted the environment and health effects of PAHs originated from residential coal combustion, and proposed an effective way by using clean coal to alleviate the associated negative impacts.

摘要

居民用煤在我国的欠发达地区仍然不可避免。清洁型煤球通常使用碱性物质,如石灰或赤泥(RM)作为添加剂,即使不改变炉灶,也有助于减少污染排放。关于赤泥清洁型煤燃烧过程中大气多环芳烃(PAHs)排放特征的研究有限。在这项研究中,通过燃烧实验研究了原煤块和清洁煤(含赤泥)中多环芳烃(PAHs)的排放因子(EFs)、来源分布和健康风险。发现烟煤和无烟煤原煤块(B-C 和 A-C)的总多环芳烃 EF 值分别为 160.1±100.9mg·kg 和 19.4±6.1mg·kg。EF 值最高的是母体多环芳烃(p-PAHs),其次是含氧多环芳烃(o-PAHs)、烷基化多环芳烃(a-PAHs)和硝基多环芳烃(n-PAHs)。B-C 和 A-C 的 p-PAHs 排放因子分别占总多环芳烃排放的 80%和 52%,而 o-PAHs 则分别占 22.9%和 44.9%,表明居民燃煤是 p-PAHs 和 o-PAHs 的重要原始来源。清洁煤是通过冷压技术与赤泥(RM)作为添加剂开发的,RM 含量为 10%的清洁煤分别称为 B-10%(烟煤)和 A-10%(无烟煤)。与原煤块相比,B-10%使 p-PAHs、o-PAHs、a-PAHs 和 n-PAHs 的 EF 值分别从 128.1、2.5、29.3mg·kg 和 161.8μg·kg 降低到 83.5、1.3、16.4mg·kg 和 102.2μg·kg,A-10%则从 10.1、0.6、8.7mg·kg 和 20.6μg·kg 降低到 11.9、0.2、2.4mg·kg 和 15.3μg·kg。5-硝基苊/苊的诊断比(煤为 0.02-0.05,生物质为 0.0002)可用于区分居民燃煤和生物质燃烧源。当 B-C 被 B-10%取代时,非致癌(男性 0.58 至 0.33,女性 1.65 至 0.95)和致癌风险(男性 5.68×10 至 2.73×10,女性 2.63×10 至 1.27×10)均有所降低。由于 6H-苯并(C,D)芘-6-酮(男性 1.74×10,女性 8.07×10)引起的致癌风险较高,o-PAHs 应引起更多关注,甚至高于 n-PAHs(男性 3.59×10,女性 1.66×10)引起的总风险。本研究结果突出了居民燃煤燃烧产生的多环芳烃对环境和健康的影响,并提出了一种通过使用清洁煤来减轻相关负面影响的有效方法。

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