Cu掺杂对硫化镍精矿制备高效异相类Fenton催化剂(Ni,Mg,Cu)Fe_(2)O_(4)的影响  

Copper doping effect on the preparation of efficient heterogeneous Fenton-like catalyst(Ni,Mg,Cu)Fe_(2)O_(4) from nickel sulfide concentrate

作　　者：刘雅贤 陈婷 韩星 张梅[1] 郭敏[1] LIU Ya-xian;CHEN Ting;HAN Xing;ZHANG Mei;GUO Min(School of Metallurgical and Ecological Engineering,University of Science and Technology Beijing,Beijing 100083,China)

机构地区：[1]北京科技大学冶金与生态工程学院,北京100083

出　　处：《工程科学学报》2021年第7期935-945,共11页Chinese Journal of Engineering

基　　金：国家自然科学基金资助项目(U1810205)。

摘　　要：以硫化镍精矿为原料,采用共沉淀–煅烧法成功制备出Cu掺杂尖晶石铁氧体(Ni,Mg,Cu)Fe_(2)O_(4)异相类Fenton催化剂.利用X射线衍射(XRD)、扫描电子显微镜(SEM)及X射线光电子能谱(XPS)等手段系统研究了Cu掺杂量对所制备产物微观结构、形貌及催化性能的影响;确立了最优催化体系为光助类Fenton催化体系“(Ni,Mg,Cu)Fe_(2)O_(4)催化剂/H2O2/可见光”,揭示了Cu掺杂对(Mg,Ni)Fe_(2)O_(4)催化活性的增强机制.结果表明:在选定的实验条件下,制备得到的产物均为纯相立方尖晶石铁氧体.当Ni与Cu摩尔比为1∶1时,合成的(Ni,Mg,Cu)Fe_(2)O_(4)在可见光照180 min条件下对质量浓度为10 mg∙L^(−1)的罗丹明B(RhB)溶液的降解率可达94.5%.究其主要原因为:随着Cu掺杂量的增加,占据(Ni,Mg,Cu)Fe_(2)O_(4)八面体位的Fe^(3+)和Cu^(2+)的相对含量增加,即裸露于铁氧体表面的Fe^(3+)和Cu^(2+)数量增多,以及两者的协同作用,加速了羟基自由基(·OH)反应的发生,最终使得RhB溶液的降解效率从73.1%提高至94.5%.Organic contaminants such as dyes and antibiotics have become the focus of water treatment research in recent years due to their complex composition,high toxicity,and difficulty in biodegradation.Spinel ferrite heterogeneous Fenton-like catalysts,with a chemical formula of MFe_(2)O_(4)(MFe_(2)O_(4),M is a divalent metallic cation or its combination,and the divalent cation is generally Ni,Zn,Mn,Co,Cu,and Mg,etc.),have attracted much attention because of their excellent structural stability and good magnetic recovery performance.However,the catalytic activity of these catalysts is not ideal and almost all the reported catalysts are synthesized by pure chemical reagents,which restrict their industrial application.Therefore,the preparation of highly efficient heterogeneous Fenton-like catalysts with low cost becomes the key to the treatment of refractory organic wastewater.In this study,copper-doped spinel ferrite(Ni,Mg,Cu)Fe_(2)O_(4) was successfully synthesized from nickel sulfide concentrate by a coprecipitation–calcination method.The effect of copper doping concentration on the structure,micro-morphology,and catalytic performance of as-prepared samples was systematically investigated by X-ray diffraction,scanning electron microscopy,and X-ray photoelectron spectroscopy.The optimal catalytic system was established as the photo-assisted Fenton-like catalytic system,“(Ni,Mg,Cu)Fe_(2)O_(4) catalyst/H2O2/visible light”,and the enhancement mechanism of copper doping on the catalytic activity of(Mg,Ni)Fe_(2)O_(4) was revealed.Results showed that all formed products were pure spinel ferrites under the selected synthesis conditions.With 1∶1 molar ratio of Ni to Cu,the formed(Ni,Mg,Cu)Fe_(2)O_(4) catalyst achieved 94.5%degradation efficiency for 10-mg∙L^(−1) RhB solution under visible light irradiation for 180 min.This observed behavior may be ascribed mainly to the increased relative contents of Fe^(3+) and Cu^(2+) ions at octahedral site.Hydroxyl radical(·OH)reaction accelerated due to increased amount of Fe

关 键 词：硫化镍精矿 Cu掺杂量 尖晶石铁氧体(Ni Mg Cu)Fe_(2)O_(4) 异相类Fenton催化剂 煅烧 

分 类 号：TF803.21[冶金工程—有色金属冶金] TB34[一般工业技术—材料科学与工程]