β-SiC粉体中常见金属杂质的亚临界水热去除工艺

硅酸盐通报 ›› 2021, Vol. 40 ›› Issue (8): 2713-2718.

β-SiC粉体中常见金属杂质的亚临界水热去除工艺

王波^1,2, 段晓波^1,2,3, 邓丽荣^1,2,3, 王嘉博^1,2,3, 陆树河^1,2,3, 王晓刚^1,2,3

1.西安科技大学材料科学与工程学院,西安 710000;
2.陕西省硅镁产业节能与多联产工程技术研究中心,西安 710000;
3.咸阳新能源材料产业技术研究院,咸阳 712000

收稿日期:2021-03-09 修回日期:2021-04-08 出版日期:2021-08-15 发布日期:2021-09-02
通讯作者: 段晓波,博士,讲师。E-mail:xiaobo12558@163.com
作者简介:王波(1995—),男,硕士研究生。主要从事高纯碳化硅粉体的研究。E-mail:waangb@qq.com
基金资助:
国家自然科学基金青年科学基金(51602254);陕西省自然科学基础研究计划(2020JQ-737);咸阳市重大科技专项计划(2019K01-13)

Subcritical Hydrothermal Removal of Common Metal Impurity in β-SiC Powder

WANG Bo^1,2, DUAN Xiaobo^1,2,3, DENG Lirong^1,2,3, WANG Jiabo^1,2,3, LU Shuhe^1,2,3, WANG Xiaogang^1,2,3

1. College of Materials Science and Engineering, Xi'an University of Science and Technology, Xi'an 710000, China;
2. Shaanxi Engineering Research Center of Energy Saving and Polygeneration in Silicon and Magnesium Industry, Xi'an 710000, China;
3. Xianyang Industrial Technology Research Institute of New Energy Materials, Xianyang 712000, China

Received:2021-03-09 Revised:2021-04-08 Online:2021-08-15 Published:2021-09-02

摘要/Abstract

摘要： 高纯β-SiC粉体作为原料,广泛应用于半导体晶圆、半导体窑具、半导体芯片设备用陶瓷器件等产品。高温高压可以促进水热反应,采用亚临界水热法可去除工业合成β-SiC粉体中的金属杂质。研究不同酸体系下β-SiC粉体中常见金属杂质的去除效果。利用电感耦合等离子原子发射光谱仪(ICP-OES)检测微量元素的含量,通过X射线衍射仪(XRD)和扫描电镜(SEM)对β-SiC粉体的物相组成和微观结构进行表征。结果表明,对于Cr和Zr去除效果较好的是HCl体系,对于Ca、Fe、Mg和Ti去除效果较好的是HCl+HF+HNO₃体系,对于Al和K去除效果较好的是H₂SO₄+(NH₄)₂SO₄体系。采用HCl体系处理的最佳反应温度为200 ℃,采用HCl+HF+HNO₃体系处理的最佳反应温度是220 ℃,采用H₂SO₄+(NH₄)₂SO₄体系处理的最佳反应温度是200 ℃。其中,H₂SO₄+(NH₄)₂SO₄体系可将β-SiC粉体中常见金属杂质含量降低至最少(杂质总含量为920.31 mg/L),因此该体系为β-SiC粉体除杂的最优方案。

关键词: β-SiC粉体, 水热法, 金属杂质, 电感耦合等离子体, 提纯

Abstract: High-purity β-SiC powders are used as raw materials for semiconductor wafers, semiconductor kiln furniture and ceramic devices used in semiconductor chip equipment. A subcritical hydrothermal method was used to remove metal impurities in β-SiC powders synthesized by high-temperature and high-pressure, which promotes the hydrothermal reaction. The removal effect of common metal impurities in β-SiC powders under different acid systems was studied. The content of trace elements was detected by inductively coupled plasma optical emission spectrometry spectrometry (ICP-OES), and the phase composition and microstructure of β-SiC powders were characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). The results are as follows: the HCl system is better for Cr and Zr removal than the other two; the HCl+HF+HNO₃ system is better for Ca, Fe, Mg and Ti, and H₂SO₄+(NH₄)₂SO₄ system is better for Al and K. The best reaction temperature for treatment with HCl system is 200 ℃, the best reaction temperature for treatment with HCl+HF+HNO₃ system is 220 ℃, and the best reaction temperature for treatment with H₂SO₄+(NH₄)₂SO₄ system is 200 ℃. Among them, H₂SO₄+(NH₄)₂SO₄ system reduces the content of common metal impurities in β-SiC powders to the minimum, and the total content of impurities is 920.31 mg/L. Therefore, H₂SO₄+(NH₄)₂SO₄ system is the optimal scheme for β-SiC powders impurity removal.

Key words: β-SiC powder, hydrothermal method, metal impurity, inductively coupled plasma, purification

中图分类号:

TQ163

王波, 段晓波, 邓丽荣, 王嘉博, 陆树河, 王晓刚. β-SiC粉体中常见金属杂质的亚临界水热去除工艺[J]. 硅酸盐通报, 2021, 40(8): 2713-2718.

WANG Bo, DUAN Xiaobo, DENG Lirong, WANG Jiabo, LU Shuhe, WANG Xiaogang. Subcritical Hydrothermal Removal of Common Metal Impurity in β-SiC Powder[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2021, 40(8): 2713-2718.

参考文献

[1] 陈勇臻.SiC单晶抛光片的制备与表征[D].西安:西安理工大学,2008.
CHEN Y Z. Preparation and characterization of polished SiC single crystal wafer[D]. Xi'an: Xi'an University of Technology, 2008 (in Chinese).
[2] ROTTNER K, FRISCHHOLZ M, MYRTVEIT T, et al. SiC power devices for high voltage applications[J]. Materials Science and Engineering: B, 1999, 61/62: 330-338.
[3] HOBGOOD H M, BRADY M, BRIXIUS W, et al. Growth and characterization of semiconductor silicon carbide for electronic and optoelectronic applications[M]//Advances in Crystal Growth Research. Amsterdam: Elsevier, 2001: 266-281.
[4] 陈之战,施尔畏,肖兵,等.原料对碳化硅单晶生长的影响[J].无机材料学报,2003,18(4):737-743.
CHEN Z Z, SHI E W, XIAO B, et al. Effects of raw materials on the growth of silicon carbide single crystal[J]. Journal of Inorganic Materials, 2003, 18(4): 737-743 (in Chinese).
[5] 邓丽荣,王晓刚,陆树河,等.多热源真空合成高纯度、高密度、大粒径3C-SiC微粉[J].中国粉体技术,2020,26(2):29-34.
DENG L R, WANG X G, LU S H, et al. Preparation of high purity, high density and large particle size 3C-SiC powder by vacuum synthesis with multiple heat sources[J]. China Powder Science and Technology, 2020, 26(2): 29-34 (in Chinese).
[6] LARCIPRETE R, LIZZIT S, CEPEK C, et al. Thermal reactions at the interface between Si and C nanoparticles: nanotube self-assembling and transformation into SiC[J]. Surface Science, 2003, 532/533/534/535: 886-891.
[7] 茆福炜.SiC微粉提纯工艺研究[D].苏州:苏州大学,2014.
MAO F W. Study on purification process of SiC micropowder[D]. Suzhou: Soochow University, 2014 (in Chinese).
[8] 赵平,张艳娇,刘广学,等.陶瓷级碳化硅微粉提纯试验研究[J].非金属矿,2009,32(4):48-50.
ZHAO P, ZHANG Y J, LIU G X, et al. Experimental study on purification of ceramic grade SiC powder[J]. Non-Metallic Mines, 2009, 32(4): 48-50 (in Chinese).
[9] 孙毅,陈亚丽,徐元清,等.高铁碳化硅微粉的处理装置及处理方法:CN201410656133.4[P].2015-03-10.
SUN Y, CHEN Y L, XU Y Q, et al. Treatment device and treatment method of high-iron silicon carbide micropowder: CN201410656133.4[P]. 2015-03-10 (in Chinese).
[10] 付仲超.工业SiC粉末的除碳除铁工艺研究[D].兰州:兰州理工大学,2013.
FU Z C. The research on removing carbon and iron from industrial silicon carbide[D]. Lanzhou: Lanzhou University of Technology, 2013 (in Chinese).
[11] 赵维国,李经文,张辛亥,等.东荣矿区煤样氧化反应动力学热分析[J].西安科技大学学报,2020,40(2):238-243.
ZHAO W G, LI J W, ZHANG X H, et al. Kinetics and thermal analysis of oxidation reaction of coal samples in Dongrong mining area[J]. Journal of Xi'an University of Science and Technology, 2020, 40(2): 238-243 (in Chinese).
[12] 孟保利,沈谦,刘妮.一种以铵离子为络合剂稳定铝合金酸洗溶液的方法:CN201610512789.8[P].2017-02-21.
MENG B L, SHEN Q, LIU N. The invention relates to a method of using ammonium ion as complexing agent to stabilize the pickling solution of aluminum alloy: CN201610512789.8[P]. 2017-02-21 (in Chinese).

[1]	王波, 段晓波, 邓丽荣, 陆树河, 王晓刚, 白枭. β-SiC粉体Si杂质的亚临界水热去除工艺[J]. 硅酸盐通报, 2021, 40(2): 591-596.
[2]	时军;王晶;史忠祥;戴丽静. 表面活性剂对YMn2O5粉体微观形貌的影响[J]. 硅酸盐通报, 2020, 39(9): 3001-3007.
[3]	孙青;柯美林;撒玉彪;张俭;严俊;盛嘉伟. 水热法制备Bi2MoO6/埃洛石复合光催化剂及其性能研究[J]. 硅酸盐通报, 2020, 39(5): 1677-1680.
[4]	李鑫;吴雪兰;龙红明;王为奎;余正伟;张洋. 低品质膨润土提质改性技术研究[J]. 硅酸盐通报, 2020, 39(3): 837-843.
[5]	赵春洋;范文强;李春庆;王永;杨红健;刘晓莉. 碱式硫酸镁晶须对氯氧镁水泥性能的影响[J]. 硅酸盐通报, 2020, 39(2): 435-439.
[6]	季鸣童;郑伟超. 水热法制备氮掺杂石墨烯水凝胶及其超电容性能研究[J]. 硅酸盐通报, 2020, 39(2): 643-648.
[7]	燕可翀, 李子鹏, 李杨敏, 王平治. 粉煤灰碱熔-水热合成沸石用于水溶液中汞的吸附[J]. 硅酸盐通报, 2020, 39(12): 3939-3944.
[8]	李瑞珍;杨建伟;张志鹏;卢金山. 大理石废料水热法制备高白度碳酸钙粉体及其晶形控制[J]. 硅酸盐通报, 2019, 38(9): 2719-272.
[9]	李倩男, 王桂玲, 张卫民, 王欣昱, 陈俊明. 多孔球状Mn3O4的制备及电容特性研究[J]. 硅酸盐通报, 2019, 38(7): 2157-2161.
[10]	谈翔;李月明;王竹梅;高轶群;沈宗洋;乐少文;濮秦衡. 以CA为络合剂水热法合成硅酸锆粉体的研究[J]. 硅酸盐通报, 2019, 38(6): 1694-169.
[11]	杨森;杨绍斌;董伟;沈丁. 天然微晶石墨提纯工艺及可逆储锂性能[J]. 硅酸盐通报, 2019, 38(4): 1148-115.
[12]	王其波;谢峻林;刘小青;李凤祥;公丕军;何峰. TiO2载体制备条件及结构对MnOx/TiO2催化剂性能的影响[J]. 硅酸盐通报, 2019, 38(3): 711-716.
[13]	焦菲;艾桃桃;罗清威;李文虎. 花状微球结构MoS2的制备及其光催化性能研究[J]. 硅酸盐通报, 2019, 38(2): 323-326.
[14]	张谦;文书明;丰奇成;聂文林;刘建. 鳞片石墨的提纯工艺研究现状与展望[J]. 硅酸盐通报, 2019, 38(2): 392-397.
[15]	刘超文;徐广通;邹亢;徐华. 介孔二氧化硅微球的制备及其形成机理探究[J]. 硅酸盐通报, 2018, 37(9): 2787-2793.