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室内通过与亚硝酸(HONO)的非均相反应广泛形成有毒的硝化双酚。

Widespread formation of toxic nitrated bisphenols indoors by heterogeneous reactions with HONO.

作者信息

Yang Diwen, Liu Qifan, Wang Sizhi, Bozorg Matin, Liu Jiabao, Nair Pranav, Balaguer Patrick, Song Datong, Krause Henry, Ouazia Boualem, Abbatt Jonathan P D, Peng Hui

机构信息

Department of Chemistry, University of Toronto, Toronto, ON, Canada.

Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.

出版信息

Sci Adv. 2022 Dec 2;8(48):eabq7023. doi: 10.1126/sciadv.abq7023.

Abstract

With numerous structurally diverse indoor contaminants, indoor transformation chemistry has been largely unexplored. Here, by integrating protein affinity purification and nontargeted mass spectrometry analysis (PUCA), we identified a substantial class of previously unrecognized indoor transformation products formed through gas-surface reactions with nitrous acid (HONO). Through the PUCA, we identified a noncommercial compound, nitrated bisphenol A (BPA), from house dust extracts strongly binding to estrogen-related receptor γ. The compound was detected in 28 of 31 house dust samples with comparable concentrations (ND to 0.30 μg/g) to BPA. Via exposing gaseous HONO to surface-bound BPA, we demonstrated it likely forms via a heterogeneous indoor chemical transformation that is highly selective toward bisphenols with electron-rich aromatic rings. We used N-nitrite for in situ labeling and found 110 nitration products formed from indoor contaminants with distinct aromatic moieties. This study demonstrates a previously unidentified class of chemical reactions involving indoor HONO, which should be incorporated into the risk evaluation of indoor contaminants, particularly bisphenols.

摘要

由于存在众多结构各异的室内污染物,室内转化化学在很大程度上尚未得到探索。在此,通过整合蛋白质亲和纯化和非靶向质谱分析(PUCA),我们鉴定出了一大类以前未被认识的室内转化产物,这些产物是通过与亚硝酸(HONO)的气-表面反应形成的。通过PUCA,我们从与雌激素相关受体γ强烈结合的室内灰尘提取物中鉴定出一种非商业化合物——硝化双酚A(BPA)。在31个室内灰尘样本中的28个样本中检测到了该化合物,其浓度与BPA相当(未检出至0.30μg/g)。通过将气态HONO暴露于表面结合的BPA,我们证明它可能是通过一种非均相室内化学转化形成的,这种转化对具有富电子芳环的双酚具有高度选择性。我们使用N-亚硝酸盐进行原位标记,发现由具有不同芳香部分的室内污染物形成了110种硝化产物。这项研究证明了一类以前未被识别的涉及室内HONO的化学反应,应将其纳入室内污染物,特别是双酚的风险评估中。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6823/10936053/27a3d85bcdad/sciadv.abq7023-f1.jpg

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