Homogeneous activation of peroxymonosulfate using a low-dosage cross-bridged cyclam manganese(II) complex for organic pollutant degradation via a nonradical pathway.,Journal of Hazardous Materials

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Homogeneous activation of peroxymonosulfate using a low-dosage cross-bridged cyclam manganese(II) complex for organic pollutant degradation via a nonradical pathway.
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2020-03-19 , DOI: 10.1016/j.jhazmat.2020.122560
Yuqing Yu ₁ , Peng Tan ₂ , Xinjue Huang ₁ , Junjie Tao ₁ , Yingying Liu ₃ , Raymond Jianxiong Zeng ₁ , Man Chen ₁ , Shungui Zhou ₁

Affiliation

The high dosage of catalyst requirement and weak anti-interference ability limit current heterogeneous manganese (Mn) catalyst/peroxymonosulfate (PMS) systems to remediate the organic polluted wastewater in complicated environment. Inspired by the concept of atom economy, herein, a homogenous manganese complex bearing a cross-bridged cyclam ligand Mn(cbc)Cl2 (MnL, L = cbc = 4,11-dimethyl-1,4,8,11-tetraazabicyclo[6.6.2]hexadecane)) is capable of activating PMS for reactive brilliant red K-2BP (RBR K-2BP) degradation. The dosage of MnL for PMS activation was low, in a range of 0.38∼3.8 mg/L. The quenching experiments demonstrated that the degradation was a nonradical-controlled process. Using methyl phenyl sulfoxide (PMSO) as a probe, the dominated degradation process of substrate was via an oxygen transfer pathway. Moreover, a high-valent Mn-oxo [(O)MnVLCl2]+ was directly detected using electrospray ionization mass spectrometry (ESI/MS). This system showed excellent anti-interference ability to both anions and humic acid, a typical natural organic matter. The atom economy, represented by an index ((mg pollutant)/h/(g catalyst)), showed that MnL 22737 in PMS activation was much higher than those of Mn-based heterogeneous catalytic systems 67∼960 and was only behind that of iron-tetraamidomacrocyclic ligand Fe-TAML 59139. This work provides insights into designing an atom-economic Mn-based PMS activator for efficient treatments for organic pollutants in a complicated environment.

中文翻译：

使用低剂量交叉桥环仙客来锰（II）配合物通过非自由基途径降解过氧单硫酸盐的均相活化。

高剂量的催化剂需求和较弱的抗干扰能力限制了目前的多相锰（Mn）催化剂/过氧单硫酸盐（PMS）系统在复杂环境中修复有机污染废水的能力。受原子经济概念的启发，本文中的均相锰配合物带有交叉桥联的Cyclam配体Mn（cbc）Cl2（MnL，L = cbc = 4,11-二甲基-1,4,8,11-四氮杂双环[6.6] .2]十六烷））能够活化PMS进行活性艳红K-2BP（RBR K-2BP）降解。用于PMS活化的MnL剂量较低，范围为0.38〜3.8 mg / L。淬灭实验表明降解是非自由基控制的过程。使用甲基苯基亚砜（PMSO）作为探针，底物的主要降解过程是通过氧转移途径。此外，使用电喷雾电离质谱法（ESI / MS）直接检测高价Mn-氧代[（O）MnVLCl2] +。该系统对阴离子和腐殖酸（一种典型的天然有机物）均具有出色的抗干扰能力。用指数（（mg污染物）/ h /（g催化剂））表示的原子经济性表明，MnS 22737在PMS活化中远高于Mn基非均相催化体系67〜960，并且仅落后于铁-四酰胺基大环配体Fe-TAML59139。这项工作为设计一种原子经济的锰基PMS活化剂提供了见识，该活化剂可有效处理复杂环境中的有机污染物。典型的天然有机物。用指数（（mg污染物）/ h /（g催化剂））表示的原子经济性表明，MnS 22737在PMS活化中远高于Mn基非均相催化体系67〜960，并且仅落后于铁-四酰胺基大环配体Fe-TAML59139。这项工作为设计一种原子经济的锰基PMS活化剂提供了见识，该活化剂可有效处理复杂环境中的有机污染物。典型的天然有机物。用指数（（mg污染物）/ h /（g催化剂））表示的原子经济性表明，MnS 22737在PMS活化中远高于Mn基非均相催化体系67〜960，并且仅落后于铁-四酰胺基大环配体Fe-TAML59139。这项工作为设计一种原子经济的锰基PMS活化剂提供了见识，该活化剂可有效处理复杂环境中的有机污染物。

更新日期：2020-03-19

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