工程科学学报，第40卷，第11期：1300-1308,2018年11月 Chinese Joural of Engineering,Vol.40,No.11:1300-1308,November 2018 DOI:10.13374/j.issn2095-9389.2018.11.003;http://journals.ustb.edu.cn 稀土金属脱除氧杂质的新技术及驱动机制研究进展 傅凯2)，李栓12)，姜晓静2)，韩丽辉3)，田文怀)四，李星国2) 1)北京科技大学材料科学与工程学院，北京1000832)北京大学化学与分子工程学院，北京100871 3)北京科技大学治金与生态工程学院，北京100083 ☒通信作者，E-mail:wenhuaitian@usth.edu.cm 摘要介绍了活泼金属除气法、等离子体熔炼法和固溶氢原子除气法等稀土金属脱除氧杂质的新方法，详细归纳了将氧杂 质含量限制在5×10~5以下的工艺条件.重点介绍新方法中引入活泼金属、氢等离子体、活性固溶氢原子等各种外部驱动因素 的设计思想，提出提纯新技术的同时探究了痕量杂质的迁移规律及去除机制，深化对杂质存在形式、行为规律及提纯机理的 认识.采用FAST-2D与Stefan数值模拟技术、O2示踪同位素标记技术，CALPHAD相图数据库模拟计算技术对稀土金属高纯 化的新工艺提供理论指导与评价，加深对提纯驱动机制的理解. 关键词稀土：高纯化：氧含量：模拟计算：机理 分类号TG146.45 Research progress on novel technology and mechanisms for the removal of oxygen impurities in rare-earth metals FU Kai2),LI Shuan'),JIANG Xiao-jing?),HAN Li-hui),TIAN Wen-huai,LI Xing-guo2) 1)School of Materials Science and Engineering,University of Science and Technology Beijing,Beijing 100083,China 2)College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China 3)School of Metallurgical and Ecological Engineering,University of Science and Technology Beijing,Beijing 100083,China Corresponding author,E-mail:wenhuaitian@ustb.edu.cn ABSTRACT Rare-earth metals play a very important role in the development of high-tech industries and the research of functional materials.The demand for high-purity rare-earth metals has rapidly increased because of the development of modern society and the rare-earth industry.However,the purity of commercial rare-earth metal materials is the key factor limiting the rapid development of rare-earth industry.The major impurities in commercial rare-earth metal materials are gas impurities,especially oxygen.The removal of oxygen impurities is extremely challenging because of their strong affinity,which causes the problem of high oxygen concentrations of raw rare-earth metal materials.Therefore,effectively removing oxygen purities is the key to achieve ultra-high purity rare-earth metals. In recent years,several new and innovative strategies to remove oxygen impurities from rare earth metals have been proposed and inves- tigated.To overcome the kinetic and thermodynamic barriers,various driving forces have been creatively introduced into the refining process.This article presented some novel purification methods to remove oxygen impurities,including active metal external getting method,hydrogen plasma arc melting method and hydrogen in-situ refining method.Experimental results show that the oxygen concen- trations in rare-earth metals can be reduced effectively by introducing various driving forces.The optimum process conditions of these techniques were introduced in detail,with the final concentrations of oxygen being reduced to below 5x10.The design concept and refining mechanism of the driving forces,including active metal,hydrogen plasma and dissolved active hydrogen atoms in rare-earth metal,were discussed systematically in this paper.The refining principle and migration mechanism of oxygen impurities were also dis- 收稿日期：2017-11-15 基金项目：国家自然科学基金资助项目(51431001,51771002，U1607126,21321001):北京市科学技术委员会资助项目(Z17110000091702)工程科学学报,第 40 卷,第 11 期:1300鄄鄄1308,2018 年 11 月 Chinese Journal of Engineering, Vol. 40, No. 11: 1300鄄鄄1308, November 2018 DOI: 10. 13374 / j. issn2095鄄鄄9389. 2018. 11. 003; http: / / journals. ustb. edu. cn 稀土金属脱除氧杂质的新技术及驱动机制研究进展 傅 凯1,2) , 李 栓1,2) , 姜晓静2) , 韩丽辉3) , 田文怀1)苣 , 李星国2) 1) 北京科技大学材料科学与工程学院, 北京 100083 2) 北京大学化学与分子工程学院, 北京 100871 3) 北京科技大学冶金与生态工程学院, 北京 100083 苣 通信作者, E鄄mail: wenhuaitian@ ustb. edu. cn 摘 要 介绍了活泼金属除气法、等离子体熔炼法和固溶氢原子除气法等稀土金属脱除氧杂质的新方法,详细归纳了将氧杂 质含量限制在 5 伊 10 - 5以下的工艺条件. 重点介绍新方法中引入活泼金属、氢等离子体、活性固溶氢原子等各种外部驱动因素 的设计思想,提出提纯新技术的同时探究了痕量杂质的迁移规律及去除机制,深化对杂质存在形式、行为规律及提纯机理的 认识. 采用 FAST鄄2D 与 Stefan 数值模拟技术、 18O2 示踪同位素标记技术、CALPHAD 相图数据库模拟计算技术对稀土金属高纯 化的新工艺提供理论指导与评价,加深对提纯驱动机制的理解. 关键词 稀土; 高纯化; 氧含量; 模拟计算; 机理 分类号 TG146郾 45 收稿日期: 2017鄄鄄11鄄鄄15 基金项目: 国家自然科学基金资助项目 (51431001, 51771002, U1607126, 21321001); 北京市科学技术委员会资助项目(Z17110000091702) Research progress on novel technology and mechanisms for the removal of oxygen impurities in rare鄄earth metals FU Kai 1,2) , LI Shuan 1,2) , JIANG Xiao鄄jing 2) , HAN Li鄄hui 3) , TIAN Wen鄄huai 1)苣 , LI Xing鄄guo 2) 1) School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China 2) College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China 3) School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China 苣 Corresponding author, E鄄mail: wenhuaitian@ ustb. edu. cn ABSTRACT Rare鄄earth metals play a very important role in the development of high鄄tech industries and the research of functional materials. The demand for high鄄purity rare鄄earth metals has rapidly increased because of the development of modern society and the rare鄄earth industry. However, the purity of commercial rare鄄earth metal materials is the key factor limiting the rapid development of rare鄄earth industry. The major impurities in commercial rare鄄earth metal materials are gas impurities, especially oxygen. The removal of oxygen impurities is extremely challenging because of their strong affinity, which causes the problem of high oxygen concentrations of raw rare鄄earth metal materials. Therefore, effectively removing oxygen purities is the key to achieve ultra鄄high purity rare鄄earth metals. In recent years, several new and innovative strategies to remove oxygen impurities from rare earth metals have been proposed and inves鄄 tigated. To overcome the kinetic and thermodynamic barriers, various driving forces have been creatively introduced into the refining process. This article presented some novel purification methods to remove oxygen impurities, including active metal external getting method, hydrogen plasma arc melting method and hydrogen in鄄situ refining method. Experimental results show that the oxygen concen鄄 trations in rare鄄earth metals can be reduced effectively by introducing various driving forces. The optimum process conditions of these techniques were introduced in detail, with the final concentrations of oxygen being reduced to below 5 伊 10 - 5 . The design concept and refining mechanism of the driving forces, including active metal, hydrogen plasma and dissolved active hydrogen atoms in rare鄄earth metal, were discussed systematically in this paper. The refining principle and migration mechanism of oxygen impurities were also dis鄄