| Cu掺杂对硫化镍精矿制备高效异相类Fenton催化剂(Ni,Mg, Cu)Fe2O4的影响 |
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| 作者姓名： | 刘雅贤 陈婷 韩星 张梅 郭敏 |
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| 作者单位： | 北京科技大学冶金与生态工程学院，北京 100083 |
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| 基金项目： | 国家自然科学基金资助项目（U1810205） |
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| 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)Fe2O4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)Fe2O4催化剂/H2O2/可见光”，揭示了Cu掺杂对(Mg, Ni)Fe2O4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)Fe2O4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)Fe2O4八面体位的Fe3+和Cu2+的相对含量增加，即裸露于铁氧体表面的Fe3+和Cu2+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%。
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| 关 键 词： | 硫化镍精矿 Cu掺杂量 尖晶石铁氧体(Ni，Mg，Cu)Fe2O4 异相类Fenton催化剂 煅烧 |
| 收稿时间： | 2020-06-18 |
Copper doping effect on the preparation of efficient heterogeneous Fenton-like catalyst(Ni,Mg,Cu)Fe2O4 from nickel sulfide concentrate |
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| Authors: | LIU Ya-xian CHEN Ting HAN Xing ZHANG Mei GUO Min |
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| Affiliation: | School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China |
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| Abstract: | 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 MFe2O4 (MFe2O4, 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)Fe2O4 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)Fe2O4 catalyst/H2O2/visible light”, and the enhancement mechanism of copper doping on the catalytic activity of (Mg, Ni)Fe2O4 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)Fe2O4 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 Fe3+ and Cu2+ ions at octahedral site. Hydroxyl radical (·OH) reaction accelerated due to increased amount of Fe3+ and Cu2+ exposed on the surface and enhanced synergetic effect between Fe3+ and Cu2+. This improved the degradation efficiency of RhB solution from 73.1% to 94.5%. |
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