Science of the Total Environment ( IF 8.2 ) Pub Date : 2020-09-17 , DOI: 10.1016/j.scitotenv.2020.142387 Xiaolei Wang , Yingzhi Ding , Dionysios D. Dionysiou , Cun Liu , Yunping Tong , Juan Gao , Guodong Fang , Dongmei Zhou
Copper-containing minerals have been extensively used in Fenton-like processes for degradation of pollutants and have exhibited great potential for environmental remediation. This work reports the first use of copper sulfide (CuS), a typical Cu-mineral, for the activation of peroxymonosulfate (PMS) for pollutant degradation; the study also elucidates the underlying mechanism of these processes. Copper sulfide effectively activated PMS to degrade diethyl phthalate (DEP). Electron paramagnetic resonance, free radical quenching, X-ray photoelectron spectroscopy, X-ray diffraction analyses and DFT calculations confirmed that ≡Cu (I)/≡Cu (II) cycling on the surface of CuS provided the main pathway to activate PMS to produce highly oxidative species. Unlike conventional sulfate radical-based PMS activation processes, hydroxyl radical (•OH) were found to be the dominant radical in the tested CuS/PMS system, which performed more efficiently than an alternative •OH-based oxidation system (CuS/H2O2) for DEP degradation. In addition, the presence of anions such Cl− and NO3− has limited inhibition effects on DEP degradation. Overall, this study provides an efficient pathway for PMS-based environmental remediation as well as a new insight into the mechanism of PMS activation by Cu-containing minerals.
中文翻译:
硫化铜对过氧一硫酸盐的有效活化以降解邻苯二甲酸二乙酯:性能,自由基的产生和机理
含铜矿物质已广泛用于类似芬顿的过程中,以降解污染物,并显示出巨大的环境修复潜力。这项工作报告了首次使用典型的铜矿物硫化铜(CuS)活化过氧单硫酸盐(PMS)来降解污染物;该研究还阐明了这些过程的潜在机制。硫化铜有效激活了PMS,以降解邻苯二甲酸二乙酯(DEP)。电子顺磁共振,自由基猝灭,X射线光电子能谱,X射线衍射分析和DFT计算证实,CuS表面上的≡Cu(I)/≡Cu(II)循环提供了激活PMS产生的主要途径高氧化性物质。与传统的基于硫酸根的PMS活化过程不同,羟基(•在被测试的CuS / PMS系统中,发现• OH)是主要的自由基,其表现出比DEP降解的替代•基于OH的氧化系统(CuS / H 2 O 2)更有效。此外,阴离子,例如Cl组成的存在-和NO 3 -拥有有限的DEP降解抑制作用。总体而言,这项研究为基于PMS的环境修复提供了一条有效途径,并为含铜矿物质激活PMS的机理提供了新见解。