Deng Jing, Ya Chen, Ge Yongjian, Cheng Yongqing, Chen Yijing, Xu Mengyuan, Wang Hongyu
College of Civil Engineering and Architecture, Zhejiang University of Technology 18 Chaowang Road, Xiacheng District Hangzhou 310014 China
RSC Adv. 2018 Jan 9;8(5):2338-2349. doi: 10.1039/c7ra07841b.
Various transition metals (Fe, Mn, Cu and Ni) were doped into ordered mesoporous CoO to synthesize CoO-composite spinels. Their formation was evidenced by transmission electronic microscopy (TEM), X-ray diffraction (XRD) and Brunauer-Emmett-Teller (BET) analysis. It was found that CoO-composite spinels could efficiently activate peroxymonosulfate (PMS) to remove enrofloxacin (ENR) and the catalytic activity followed the order CoO-CuCoO > CoO-CoMnO > CoO-CoFeO > CoO-NiCoO. Moreover, through the calculation of the specific apparent rate constant ( ), it can be proved that the Co and Cu ions had the best synergistic effect for PMS activation. The CoO-composite spinels presented a wide pH range for the activation of PMS, but strong acidic and alkaline conditions were detrimental to ENR removal. Higher reaction temperature could promote the PMS activation process. Sulfate radical was identified as the dominating reactive species in CoO-composite spinel/PMS systems through radical quenching experiments. Meanwhile, the probable mechanisms concerning CoO-composite spinel activated PMS were proposed.
将各种过渡金属(铁、锰、铜和镍)掺杂到有序介孔氧化钴中,以合成氧化钴复合尖晶石。通过透射电子显微镜(TEM)、X射线衍射(XRD)和布鲁诺尔-埃米特-泰勒(BET)分析证实了它们的形成。研究发现,氧化钴复合尖晶石能够有效活化过一硫酸盐(PMS)以去除恩诺沙星(ENR),其催化活性顺序为CoO-CuCoO > CoO-CoMnO > CoO-CoFeO > CoO-NiCoO。此外,通过计算比表观速率常数( ),可以证明钴离子和铜离子对PMS活化具有最佳的协同效应。氧化钴复合尖晶石在较宽的pH范围内均可活化PMS,但强酸性和强碱性条件不利于ENR的去除。较高的反应温度可促进PMS的活化过程。通过自由基猝灭实验确定硫酸根自由基是氧化钴复合尖晶石/PMS体系中的主要活性物种。同时,提出了氧化钴复合尖晶石活化PMS的可能机制。