摘要
对铝(Al)和二氨基马来腈(C_4H_4N_4)的混合物分别进行等离子体辅助球磨和普通球磨,研究等离子体辅助球磨活化对合成AlN的作用机制。结果表明:相对于普通球磨,等离子体辅助球磨更有利于Al粉的晶粒细化和晶格畸变,并有利于形成Al-C_4H_4N_4纳米级的复合结构。辅助球磨中的等离子体促进C_4H_4N_4的脱胺,使C_4H_4N_4分解出更多的游离含N基团,加速与活化的Al合成AlN,辅助球磨14 h后AlN的转化率达到91%,远高于普通球磨合成AlN的产率83%。等离子体辅助球磨8 h的Al+C_4H_4N_4前驱体发生氮化反应的激活能为353.46 kJ/mol,在Ar中于800℃保温1 h可以通过固-固反应机制全部转化为超细AlN,而普通球磨8 h的前驱体反应激活能高达441.21 kJ/mol,Al需熔化后才能进行氮化反应,导致部分C_4H_4N_4先行受热分解蒸发,AlN产率仅为86%。辅助球磨促进AlN合成的主要原因是等离子体放电的高频脉冲轰击和瞬态"电火花"对粉体产生协同球磨作用。
The synthesis mechanism of AlN from diaminomaleonitrile（C4H4N4） and aluminum（Al） by using plasma assisted ball milling（PM） was investigated, in which the conventional ball milling（CM） was also used under the same conditions for comparison. The results indicate that PM is much more favorable for the grain refinement and lattice distortion of Al, as compared with that of CM, which promotes the synthesis of nanocomposite structure between Al and C4H4N4. During the process, the plasma formed in PM can promote the deammoniation of C4H4N4 to decompose much more free N-containing groups than that of the CM, which accelerates to react with the activated Al powders. After 14 h milling, the conversion rate of AlN by using PM method is up to 91%, which is much higher than the value of 83% in CM process. Furthermore, a lower nitriding reaction activation energy（353.46 kJ/mol） was obtained in the Al＋C4H4N4 precursors by 8 h-PM process, which could achieve a full conversion temperature is about 800 ℃, but for the 8 h-CM process, a higher nitriding reaction activation energy（441.21 kJ/mol） needs a higher nitriding temperature in the Al＋C4H4N4 precursors, leading to the melting of Al phase and evaporation of part of C4H4N4, and obviously reducing the conversion rate to 86%. The main synthesis mechanisms of AlN through the plasma assisted ball milling is a synergistic effect between high frequency pulse bombardment and transient ＂spark＂ on the powders by plasma discharge.
作者
杨卓立
廖海峰
孙迪
戴乐阳
刘志杰
王文春
YANG Zhuo-li;LIAO Hai-feng;SUN Di;DAI Le-yang;LIU Zhi-jie;WANG Wen-chun(Fujian Provincial Key Laboratory of Naval Architecture and Ocean Engineering,Institute of Marine Engineering,Jimei University,Xiamen 361021,China;Fujian Engineering Research Center of Ship Detecting and Remanufacturing,Xiamen 361021,China;Key Lab of Materials Modification,Ministry of Education,Dalian University of Technology,Dalian 116024,China)
出处
《中国有色金属学报》
EI
CAS
CSCD
北大核心
2018年第8期1587-1596,共10页
The Chinese Journal of Nonferrous Metals
基金
国家自然科学基金资助项目(51177008
51779103)
福建省科技计划项目(2018H0026)
福建省科技(文化)拥军项目(2016)
厦门市科技计划项目(3502Z20173031)~~
关键词
二氨基马来腈
ALN
等离子辅助球磨
固-固反应
活化
diaminomaleonitrile
AlN
plasma assisted ball milling
solid-solid reaction
activation
