Fang Xingyu, Gan Lu, Wang Linjie, Gong Han, Xu Lijie, Wu Ying, Lu Haiqin, Han Shuguang, Cui Juqing, Xia Changlei
College of Materials Science and Engineering, Nanjing Forestry University, Nanjing, 210037 Jiangsu, People's Republic of China.
College of Materials Science and Engineering, Nanjing Forestry University, Nanjing, 210037 Jiangsu, People's Republic of China.
J Hazard Mater. 2021 Oct 5;419:126363. doi: 10.1016/j.jhazmat.2021.126363. Epub 2021 Jun 9.
In this study, mixed metal cobalt zinc oxide embedded nitrogen enriched porous carbon composites (CoZnO-PC) were prepared via pyrolyzing polyvinylpyrrolidone (PVP) encapsulated Co, Zn-bimetal centered zeolitic imidazolate frameworks (ZIF). The prepared composites were then used to activate peroxymonosulfate (PMS) for bisphenol A (BPA) removal in water. When mole ratio of Co/Zn was 2/1, the resulted CoZnO-PC possessed spinel structure with prominent degradation capability, in which the introduction of Zn accelerated the PMS activation performance of Co through establishing bimetal synergistic interactions. Both radical and non-radical activation pathways were existed in the CoZnO-PC/PMS system, in which CoZnO dominated the radical pathway whereas PC dominated the non-radical way. Since PVP contained abundant nitrogen atoms and could form strong coordination interactions with the ZIF precursor, the introduction of PVP in the ZIF precursor prevented pore collapsing during pyrolysis process, as well as enhancing the nitrogen content in the pyrolzed composites, which significantly promoted the generation of singlet oxygen. With combined pathways, the CoZnO-PC/PMS system showed a wide pH application range with promising mineralization rate. Meanwhile, the spinel-structured CoZnO-PC was magnetically separable with desirable recyclability. This study presents a novel composite with remarkable performance for the removal of refractory organic pollutants in municipal wastewater.
在本研究中,通过热解聚乙烯吡咯烷酮(PVP)封装的以钴、锌双金属为中心的沸石咪唑酯骨架(ZIF)制备了混合金属钴锌氧化物嵌入富氮多孔碳复合材料(CoZnO-PC)。然后将制备的复合材料用于活化过一硫酸盐(PMS)以去除水中的双酚A(BPA)。当钴/锌的摩尔比为2/1时,所得的CoZnO-PC具有尖晶石结构,具有显著的降解能力,其中锌的引入通过建立双金属协同相互作用加速了钴对PMS的活化性能。CoZnO-PC/PMS体系中同时存在自由基和非自由基活化途径,其中CoZnO主导自由基途径,而PC主导非自由基途径。由于PVP含有丰富的氮原子且能与ZIF前驱体形成强配位相互作用,在ZIF前驱体中引入PVP可防止热解过程中孔塌陷,同时提高热解复合材料中的氮含量,显著促进单线态氧的产生。通过联合途径,CoZnO-PC/PMS体系显示出较宽的pH应用范围和良好的矿化率。同时,尖晶石结构的CoZnO-PC具有磁分离性和理想的可回收性。本研究提出了一种新型复合材料,在去除城市废水中的难降解有机污染物方面具有卓越性能。