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室内表面和灰尘上化学污染物的羟基自由基氧化作用

Hydroxyl radical oxidation of chemical contaminants on indoor surfaces and dust.

作者信息

Fahy William D, Gong Yufeng, Wang Shenghong, Zhang Zhizhen, Li Li, Peng Hui, Abbatt Jonathan P D

机构信息

Department of Chemistry, University of Toronto, Toronto, ON M5S 3H6, Canada.

College of Marine Life Sciences, Ocean University of China, Qingdao, Shandong 266003, China.

出版信息

Proc Natl Acad Sci U S A. 2024 Nov 5;121(45):e2414762121. doi: 10.1073/pnas.2414762121. Epub 2024 Oct 28.

Abstract

Humans are widely exposed to semivolatile organic contaminants in indoor environments. Many contaminants have long lifetimes following partitioning to the large surface reservoirs present indoors, which leads to long exposure times to gas-phase oxidants and multiphase chemistry. Studies have shown selective multiphase oxidation of organics on indoor surfaces, but the presence of hydroxyl radicals with nonselective reactivity and evidence of multiphase OH radical reactivity toward common indoor contaminants indicates that there may be additional unknown transformation chemistry indoors. We screened genuine indoor samples for 60 OH radical oxidation products of the common plasticizer and endocrine-disrupting contaminant bis(2-ethylhexyl) phthalate (DEHP) identified in laboratory experiments using nontargeted high-resolution mass spectrometry. At least 30 and 10 of these products are observed in indoor dust and DEHP films exposed to ambient indoor conditions, respectively, indicating that multiphase OH reactions occur indoors. Using the PROTEX model and a multimedia indoor chemical fate model, we demonstrate that these products have long indoor lifetimes and cause a higher potential for human exposure than DEHP. Some of these products are more active endocrine disruptors than DEHP itself, but most have unknown toxicities. Coexposure to all oxidation products will likely have an additive effect, leading to higher human health risks from indoor organic contaminants than previously thought. Due to the nonselective reactivity of OH radicals, it is likely that most indoor contaminants follow similar chemistry, and further study is needed to understand the prevalence and human health implications of such multiphase chemistry.

摘要

人类在室内环境中广泛接触到半挥发性有机污染物。许多污染物在分配到室内存在的大表面积储库后具有较长的寿命,这导致气相氧化剂和多相化学反应的暴露时间延长。研究表明室内表面存在有机物的选择性多相氧化,但具有非选择性反应性的羟基自由基的存在以及多相羟基自由基对常见室内污染物的反应性证据表明,室内可能还存在其他未知的转化化学过程。我们使用非靶向高分辨率质谱法,对实验室实验中鉴定出的常见增塑剂和内分泌干扰污染物邻苯二甲酸二(2-乙基己基)酯(DEHP)的60种羟基自由基氧化产物,筛选了真实的室内样品。分别在暴露于室内环境条件的室内灰尘和DEHP薄膜中观察到至少30种和10种这些产物,表明室内发生了多相羟基反应。使用PROTEX模型和室内多介质化学归宿模型,我们证明这些产物在室内具有较长的寿命,并且与DEHP相比,对人类暴露的潜在风险更高。其中一些产物是比DEHP本身更具活性的内分泌干扰物,但大多数具有未知的毒性。同时暴露于所有氧化产物可能会产生累加效应,导致室内有机污染物对人类健康造成比以前认为的更高风险。由于羟基自由基的非选择性反应性,很可能大多数室内污染物遵循类似的化学过程,需要进一步研究以了解这种多相化学的普遍性及其对人类健康的影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a172/11551331/fa67ba84afb3/pnas.2414762121fig01.jpg

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