Wang Yanhao, Sun Yunlong, Gao Mengchun, Xin Yanjun, Zhang Guangshan, Xu Peng, Ma Dong
Key Lab of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China; College of Resource and Environment, Qingdao Agricultural University, Qingdao 266109, China.
College of Resource and Environment, Qingdao Agricultural University, Qingdao 266109, China.
J Hazard Mater. 2023 Oct 5;459:132199. doi: 10.1016/j.jhazmat.2023.132199. Epub 2023 Aug 1.
Activated peroxymonosulfate (PMS) processes have emerged as an efficient advanced oxidation process to eliminate refractory organic pollutants in water. This study synthesized a novel spherical manganese oxide catalyst (0.4KBr-β-MnO) via a simple KBr-guided approach to activate PMS for degrading dimethyl phthalate (DMP). The 0.4KBr-β-MnO/PMS system enhanced DMP degradation under different water quality conditions, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine β-MnO by 8.5 times. Mn(V) was the dominant reactive species that was revealed by the generation of methyl phenyl sulfone from methyl phenyl sulfoxide oxidation. The selectivity of Mn(V) was demonstrated by the negligible inhibitory effects of Inorganic anions. Theoretical calculations confirmed that Mn (V) was more prone to attack the CO bond of the side chain of DMP. This study revealed the indispensable roles of high-valent manganese species in DMP degradation by the 0.4KBr-β-MnO/PMS system. The findings could provide insight into effective PMS activation by Mn-based catalysts to efficiently degrade pollutants in water via the high-valent manganese species.
活化过一硫酸盐（PMS）工艺已成为一种高效的高级氧化工艺，用于去除水中的难降解有机污染物。本研究通过一种简单的KBr引导方法合成了一种新型球形氧化锰催化剂（0.4KBr-β-MnO），以活化PMS降解邻苯二甲酸二甲酯（DMP）。0.4KBr-β-MnO/PMS体系在不同水质条件下均能增强DMP的降解，表现出超高且稳定的催化活性，比等量的原始β-MnO性能高出8.5倍。通过苯甲亚砜氧化生成苯甲砜揭示了Mn(V)是主要的活性物种。无机阴离子的抑制作用可忽略不计，证明了Mn(V)的选择性。理论计算证实，Mn(V)更容易攻击DMP侧链的CO键。本研究揭示了高价锰物种在0.4KBr-β-MnO/PMS体系降解DMP中的不可或缺作用。这些发现可为基于锰的催化剂有效活化PMS以通过高价锰物种高效降解水中污染物提供见解。
