The High-Effective Catalytic Degradation of Benzo[a]pyrene by Mn-Corrolazine Regulated by Oriented External Electric Field: Insight From DFT Study.
The High-Effective Catalytic Degradation of Benzo[a]pyrene by Mn-Corrolazine Regulated by Oriented External Electric Field: Insight From DFT Study.
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DOI：
10.3389/fchem.2022.884105
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发表时间：
2022
影响因子：
5.5
通讯作者：
Zhu, Chun
中科院分区：
文献类型：
--
作者：
Long, Tairen;Wan, Haiyan;Zhang, Jianqiang;Wu, Jie;Liang, Jin-Xia;Zhu, Chun
关键词：
采用第一性原理计算方法，系统研究了Mn-康拉嗪降解BaP生成羟基苯并[a]芘的过程及定向外电场（OEEF）对其的调控.广泛的密度泛函计算表明，苯并[a]芘的降解由锰corrolazine发生通过一个三步过程中，在OEEF的情况下，其中更有毒和更稳定的环氧化物中间体的产生。然而，当OEEF沿着本征Mn-O反应轴应用时，BaP降解为羟基苯并[a]芘的过程大大简化。随着OEEF强度的增加，Mn-OO corrolazine的末端O原子上的负电荷增加。随着OEEF的强度增加超过0.004 a. u，带负电荷的末端O原子具有直接夺取BaP中带正电荷的H原子的能力，BaP降解为羟基苯并[a]芘可以通过一步过程完成，避免了产生毒性更大的环氧中间体。
The degradation of BaP into hydroxybenzo[a]pyrene by Mn-corrolazine and its regulation by an oriented external electronic field (OEEF) were systematically studied using first-principle calculations. Extensive density function calculations showed that the degradation of BaP into hydroxybenzo[a]pyrene by Mn-corrolazine occurs via a three-step process in the absence of OEEF, in which a more toxic and stable epoxide intermediate is generated. However, upon application of OEEF along the intrinsic Mn-O reaction axis, the degradation of BaP into hydroxybenzo[a]pyrene is greatly simplified. The negative charge on the terminal O atom of Mn-OO corrolazine increases with an increase in the OEEF intensity. As the intensity of the OEEF increases over 0.004 a.u., the negatively charged terminal O atom has the ability to directly abstract the positively charged H atom of BaP and the degradation of BaP into hydroxybenzo[a]pyrene can be completed via a one-step process, avoiding the production of more toxic epoxide intermediates.
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