Fu Zhiqiang, Chen Jingwen, Wang Yong, Hong Huixiao, Xie Hongbin
a Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology , Dalian University of Technology , Dalian , China.
b State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP) , Chinese Academy of Sciences , Lanzhou , China.
J Environ Sci Health C Environ Carcinog Ecotoxicol Rev. 2018;36(4):272-291. doi: 10.1080/10590501.2018.1537564. Epub 2018 Nov 20.
The metabolic fate and toxicokinetics of organic phosphorus flame retardants catalyzed by cytochrome P450 enzymes (CYPs) are here investigated by in silico simulations, leveraging an active center model to mimic the CYPs, triphenyl phosphate (TPHP), tris(2-butoxyethyl) phosphate and tris(1,3-dichloro-2-propyl) phosphate as substrates. Our calculations elucidated key main pathways and predicted products, which were corroborated by current in vitro data. Results showed that alkyl OPFRs are eliminated faster than aryl and halogenated alkyl-substituted OPFRs. In addition, we discovered a proton shuttle pathway for aryl hydroxylation of TPHP and P = O bond-assisted H-transfer mechanisms (rather than nonenzymatic hydrolysis) that lead to O-dealkylation/dearylation of phosphotriesters.
本文通过计算机模拟,利用活性中心模型模拟细胞色素P450酶(CYPs),以磷酸三苯酯(TPHP)、三(2-丁氧基乙基)磷酸酯和三(1,3-二氯-2-丙基)磷酸酯为底物,研究了CYPs催化的有机磷阻燃剂的代谢命运和毒代动力学。我们的计算阐明了关键的主要途径并预测了产物,这些结果得到了当前体外数据的证实。结果表明,烷基有机磷阻燃剂的消除速度比芳基和卤代烷基取代的有机磷阻燃剂更快。此外,我们发现了TPHP芳基羟基化的质子穿梭途径以及导致磷酸三酯O-脱烷基化/脱芳基化的P=O键辅助H转移机制(而非非酶水解)。