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首页> 外文期刊>RSC Advances >Degradation of one-side fully-chlorinated 1,2,3,4-tetrachloronaphthalene over Fe–Al composite oxides and its hypothesized reaction mechanism
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Degradation of one-side fully-chlorinated 1,2,3,4-tetrachloronaphthalene over Fe–Al composite oxides and its hypothesized reaction mechanism

机译：Fe-Al复合氧化物上一侧完全氯化的1,2,3,4-四氯萘的降解及其假想反应机理

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The degradation of 1,2,3,4-tetrachloronaphthalene (CN-27) featuring a one-side fully-chlorinated aromatic ring, was evaluated over three of the prepared rod-like Fe–Al composite oxides (FeAl-1, FeAl-5 and FeAl-10). The results showed that their reactive activities were in the order of FeAl-5 ≈ FeAl-10 ? FeAl-1, which could be attributed to their different pore structural properties and reactive sites caused by the different phase interaction between iron species and the γ-Al2O3. The generation of trichloronaphthalenes (1,2,3-TrCN and 1,2,4-TrCN, i.e. CN-13 and CN-14), dichloronaphthalenes (1,2-DiCN, 1,3-DiCN, 1,4-DiCN and 2,3-DiCN, i.e. CN-3, CN-4, CN-5 and CN-10) and monochloronaphthalenes (1-MoCN and 2-MoCN, i.e. CN-1 and CN-2) suggested the occurrence of successive hydrodechlorination reactions. The amount of CN-14 exceeded that of CN-13 from 71.5% to 77.7% across the three different systems, revealing the preferred occurrence of the first hydrodechlorination step at the β-position. This is dissimilar to the preference at the α-position observed during the dechlorination of octachloronaphthalene (CN-75) over microano Fe3O4. The structural differences between one-side and two-side fully-chlorinated aromatic rings would have a pronounced impact on the reactivity of the chlorine substitution position. The major hydrodechlorination pathway was judged to be CN-27 → CN-14 → CN-4 → CN-2. Additionally, the detected 1,2,3,4,6-pentachloronaphthalene (CN-50) and 1,2,4,6/7-tetrachloronaphthalenes (CN-33/34) suggested the reverse chlorination reaction also happened while the hydrodechlorination reaction was occurring. The C–Cl bond dissociation energies (BDEs) of the parent and daughter polychlorinated naphthalene (PCN) congener were calculated using density functional theory (DFT), to achieve a deeper understanding of a different product yield distribution.
机译：在制备的三种棒状Fe–Al复合氧化物（FeAl-1，FeAl-，三价铁，三价铁和三价铁）中评估了具有一侧完全氯化芳环的1,2,3,4-四氯萘（CN-27）的降解情况。 5和FeAl-10）。结果表明，它们的反应活性为FeAl-5≈FeAl-10？ FeAl-1，可能是由于铁物种与γ-Al 2 O 之间的不同相间相互作用而导致的孔结构性质和反应位点不同所致 3 。三氯萘（1,2,3-TrCN和1,2,4-TrCN， ie CN-13和CN-14），二氯萘（1,2-DiCN，1,3- DiCN，1,4-DiCN和2,3-DiCN，即 CN-3，CN-4，CN-5和CN-10）和一氯萘（1-MoCN和2-MoCN，< em> ie CN-1和CN-2）提示了连续加氢脱氯反应的发生。在三个不同的系统中，CN-14的含量从CN-13的71.5％增至77.7％，表明在β位置发生了第一个加氢脱氯步骤是优选的。这与八氯萘（CN-75）脱氯过程中在微/纳米Fe 3 O 4上在α-位置的偏好不同 。一侧和两侧的完全氯化芳环之间的结构差异将对氯取代位置的反应性产生显着影响。判断主要的加氢脱氯途径为CN-27→CN-14→CN-4→CN-2。另外，检测到的1,2,3,4,6-五氯萘（CN-50）和1,2,4,6 / 7-四氯萘（CN-33 / 34）表明，在加氢脱氯反应中还发生了逆氯化反应。正在发生。使用密度泛函理论（DFT）计算了母体和子体多氯萘（PCN）同类物的C-Cl键解离能（BDE），以更深入地了解不同产品的产率分布。

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