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
Department of Chemistry, University of Toronto, Toronto, ON, Canada.
Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
Sci Adv. 2022 Dec 2;8(48):eabq7023. doi: 10.1126/sciadv.abq7023.
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.
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。