B-C-N化合物新相的冲击波合成

王俊莉; 刘福生; 包兴明; 彭小娟; 马海云

doi:10.11858/gywlxb.2014.01.005

B-C-N化合物新相的冲击波合成

doi: 10.11858/gywlxb.2014.01.005

王俊莉^1,,
刘福生^1,*, ,,
包兴明^{1, 2},
彭小娟¹,
马海云¹

1.
西南交通大学高压科学与技术实验室，四川成都 610031
2.
四川理工学院物理系，四川自贡 643000

基金项目: 国家自然科学基金(10874141)；西南交通大学中央高校专项基金

详细信息

作者简介:
王俊莉(1984-), 女, 硕士, 主要从事高温高压下新材料的合成研究.E-mail:wangjunli626@126.com

通讯作者:
刘福生(1966-), 男, 研究员, 博士生导师, 主要从事高压凝聚态物理、原子与分子物理以及冲击波技术研究.E-mail: fusheng_l@souhu.com

中图分类号: O521.2
计量
- 文章访问数: 7509
- HTML全文浏览量: 2223
- PDF下载量: 311
出版历程
- 收稿日期: 2012-01-09
- 修回日期: 2013-09-27

Shock Synthesis of a New B-C-N Compound

1.
Key Laboratory of High Pressure Science and Technology, Southwest Jiaotong University, Chengdu 610031, China
2.
Department of Physics, Sichuan University of Science and Engineering, Zigong 643000, China

摘要

摘要: 理论预言，B-C-N化合物可能存在多种结构，并具有优良的物理性能，因此其合成研究引起了各国学者的关注。运用二级轻气炮冲击加载与样品回收技术，在40 GPa压力附近探索了B-C-N化合物的新相合成条件。X射线衍射、高分辨率透射电镜、电子衍射、X射线光电子能谱等检测技术的分析结果表明，3种不同原子比例的B-C-N前驱物在40 GPa的强冲击合成条件下，均能生成一种新的B-C-N致密新相单晶体，尺寸约为60 nm。具有这种结构的B-C-N化合物在文献中未见报道。研究结果对进一步探索B-C-N新相的结构形态及其高温高压合成条件具有参考意义，也为理论工作者提供了一种新的B-C-N结构模型。
- B-C-N化合物 /
- 超硬材料 /
- 冲击合成 /
- 轻气炮
Abstract: Theory predicts that B-C-N compounds may exist in many structural forms and have excellent physical properties.Synthesis of such materials is attracting the attentions of scientists.A two-stage light-gas gun and the corresponding shock-recovery technology were applied to explore the synthesis conditions of B-C-N compound of new phase structures under 40 GPa pressure.XRD (X-ray diffraction), HRTEM (high-resolution transmission electron microscopy), ED (electron diffraction) and XPS (X-ray photoelectron spectroscopy) analysis show that all three precursors with different atomic ratio of B, C and N can generate a new dense phase of B-C-N compound under strong shock loading of 40 GPa.Single crystals of 60 nm are directly observed in the recovery sample.The new B-C-N compound of such structure has not been reported in the literature before.Therefore, this discovery is of significance for exploring new structures of B-C-N compounds and the synthesis conditions in future; meanwhile, a new structure of B-C-N compound is waiting to be studied by theoretical researchers.
- B-C-N compounds /
- superhard material /
- shock wave synthesis /
- light gas gun

HTML全文

图 1 冲击前3种前驱物的XRD谱

Figure 1. XRD patterns of three precursors before shock

下载: 全尺寸图片幻灯片

图 2 冲击合成实验装置示意图

Figure 2. Schematic of shock experimental facility

下载: 全尺寸图片幻灯片

图 3 强冲击压缩后回收样品的XRD谱

Figure 3. XRD patterns of the shock recovery sample

下载: 全尺寸图片幻灯片

图 4 样品Ⅱ与β-C₃N₄^[18]的XRD谱比较

Figure 4. Comparison of XRD patterns between sample Ⅱ and β-C₃N₄^[18]

下载: 全尺寸图片幻灯片

图 5 冲击回收样品Ⅲ的XPS谱

Figure 5. XPS spectra of post-shock sample Ⅲ

下载: 全尺寸图片幻灯片

图 6 冲击回收样品Ⅱ的HRTEM及ED图像

Figure 6. HRTEM image and ED pattern of the post-shock sample Ⅱ

下载: 全尺寸图片幻灯片

表 1 B-C-N冲击合成的前驱物

Table 1. Pyrolysis precursor for shock synthesis of B-C-N

Sample	m_H₃BO₃:m_C₃N₆H₆	Full width at half maximum/(°)	Product color	x_B:x_C:x_N
Ⅰ	1:2	12.0	Black	28:50:22
Ⅱ	1:1	7.8	Tawny	41:25:34
Ⅲ	2:1	7.5	White	29:53:18

下载: 导出CSV

表 2 样品的实验条件和冲击压力

Table 2. Experimental conditions and shock pressure of samples

Sample	Initial density/(g/cm³)	Impact velocity/(km/s)	Shock pressure/(GPa)	Shock temperature/(K)
Ⅰ	6.68	1.70	40	2 200
Ⅱ	6.59	1.70	40	2 300
Ⅲ	6.43	1.70	40	2 500

下载: 导出CSV

参考文献(22)

[1]	Cheng Y C, Wu X L, Li S H, et al. Ab initio determination of lattice dynamics and thermodynamics of β-BC₂N[J]. Solid State Commun, 2008, 146(1/2): 69-72. http://www.mendeley.com/research/ab-initio-determination-lattice-dynamics-thermodynamics-bbc2n/
[2]	Langenhorst F, Solozhenko V L. ATEM-EELS study of new diamond-like phases in the B-C-N system[J]. Phys Chem Chem Phys, 2002, 4(20): 5183-5188. doi: 10.1039/B206691B
[3]	Wu B R, Huang Z Q, Su W S, et al. Atomic structure and mechanical properties of BC₂N superlattice[J]. Diam Relat Mater, 2010, 19(11): 1341-1347. doi: 10.1016/j.diamond.2010.06.022
[4]	Sun H, Jhi S H, Roundy D, et al. Structural forms of cubic BC₂N[J]. Phys Rev B, 2001, 64(9): 094108. doi: 10.1103/PhysRevB.64.094108
[5]	Zhang Y, Sun H, Chen C. Superhard cubic BC₂N compared to diamond[J]. Phys Rev Lett, 2004, 93(19): 195504. doi: 10.1103/PhysRevLett.93.195504
[6]	Luo X G, Guo X J, Xu B, et al. Body-centered superhard BC₂N phases from first principles[J]. Phys Rev B, 2007, 76(9): 094103. doi: 10.1103/PhysRevB.76.094103
[7]	Caretti I, Jimenez I, Albella J M. BCN films with controlled composition obtained by the interaction between molecular beams of B and C with nitrogen ion beams[J]. Diam Relat Mater, 2003, 12: 1079-1083. doi: 10.1016/S0925-9635(02)00276-5
[8]	Mannan M A, Noguchi H, Kida T, et al. Growth and characterization of stoichiometric BCN films on highly oriented pyrolytic graphite by radiofrequency plasma enhanced chemical vapor deposition[J]. Thin Solid Films, 2010, 518(15): 4163-4169. doi: 10.1016/j.tsf.2009.11.086
[9]	Nakano S, Akaishi M, Sasaki T, et al. Segregative crystallization of several diamond-like phases from the graphitic BC₂N without an additive at 7.7 GPa[J]. Chemistry Mater, 1994, 6(12): 2246-2251. doi: 10.1021/cm00048a011
[10]	Solozhenko V L, Andrault D, Fiquet G, et al. Synthesis of superhard cubic BC₂N[J]. Appl Phys Lett, 2001, 78(10): 1385-1387. doi: 10.1063/1.1337623
[11]	何巨龙, 田永君, 于栋利, 等.高压合成B-C-N化合物的结构表征[J].硅酸盐学报, 2002, 30(1): 51-56. http://www.cqvip.com/Main/Detail.aspx?id=6018634 He J L, Tian Y J, Yu D L, et al. Structure characterization of high-pressure-synthesized B-C-N compounds[J]. Journal of the Chinese Ceramic Society, 2002, 30(1): 51-56. (in Chinese) http://www.cqvip.com/Main/Detail.aspx?id=6018634
[12]	胡文涛.晶态BCN化合物的高温高压合成及其热膨胀性质[D].秦皇岛: 燕山大学, 2004. Hu W T. Synthesis of crystalline BCN compounds under high pressure and high temperature and their thermal expansion property[D]. Qinhuangdao: Yanshan University, 2004. (in Chinese)
[13]	穆云超.硼碳氮晶体的制备工艺研究[D].郑州: 郑州大学, 2006. Mu Y C. Research for boron carbonitride crystals preparation[D]. Zhengzhou: Zhengzhou University, 2006. (in Chinese)
[14]	白锁柱. BCN化合物的合成、表征和性能[D].长春: 吉林大学, 2005. Bai S Z. Synthesis, characterization and properties of boron carbon nitride compounds[D]. Changchun: Jilin University, 2005. (in Chinese)
[15]	李雪飞, 张剑, 沈龙海, 等.六角相硼碳氮化合物的合成研究[J].高压物理学报, 2007, 21(3): 237-241. http://d.wanfangdata.com.cn/Periodical/gywlxb200703003 Li X F, Zhang J, Shen L H, et al. Synthesis and characterization of h-BCN nanocrystallite under high-pressure and high-temperature[J]. Chinese Journal of High Pressure Physics, 2007, 21(3): 237-241. (in Chinese) http://d.wanfangdata.com.cn/Periodical/gywlxb200703003
[16]	杨建, 丘泰, 沈春英, 等.先驱体热解制备富硼、氮BCN化合物及其发光性能研究[J].无机材料学报, 2009, 24(1): 13-17. http://www.cqvip.com/QK/93432X/200901/29194693.html Yang J, Qiu T, Shen C Y, et al. Photoluminescence of(boron and nitrogen)-rich BCN compounds pyrolysed from precursor[J]. Joumal of Inorganic Materials, 2009, 24(1): 13-17. (in Chinese) http://www.cqvip.com/QK/93432X/200901/29194693.html
[17]	Matizamhuka W R. A study on the synthesis of ultrahard cubic BC₂N heterodiamond[D]. Johannesburg, South Africa: University of the Witwatersrand, 2010.
[18]	马海云, 刘福生, 李永宏, 等.强冲击压缩条件下g-C₃N₄向β-C₃N₄直接转化[J].高压物理学报, 2012, 26(3): 319-324. http://www.cnki.com.cn/Article/CJFDTotal-GYWL201203014.htm Ma H Y, Liu F S, Li Y H, et al. Strong shock-compression of g-C₃N₄ precursor for direct synthesis of β-C₃N₄[J]. Chinese Journal of High Pressure Physics, 2012, 26(3): 319-324. (in Chinese) http://www.cnki.com.cn/Article/CJFDTotal-GYWL201203014.htm
[19]	白锁柱, 姚斌, 黄保坤, 等. BCN化合物的合成与表征[J].高等学校化学学报, 2005, 26(5): 811-815. http://www.cqvip.com/Main/Detail.aspx?id=20722950 Bai S Z, Yao B, Huang B K, et al. Preparation and characterization of BCN[J]. Chemical Journal of Chinese Universities, 2005, 26(5): 811-815. (in Chinese) http://www.cqvip.com/Main/Detail.aspx?id=20722950
[20]	经福谦.实验物态方程导引[M].第2版.北京: 科学出版社, 1999: 199-200. Jing F Q. Introduction to Experimental Equation of State[M]. 2nd Ed. Beijing: Science Press, 1999: 199-200. (in Chinese)
[21]	Onodera A, Matsumoto K, Hirai T, et al. Synthesis of dense forms of B-C-N system using chemical-vapor-deposition/high-pressure process[J]. J Mater Sci, 2001, 36(3): 679-684. doi: 10.1023/A:1004832807084
[22]	Watanabe M O, Itoh S, Mizushima K, et al. Bonding characterization of BC₂N thin films[J]. Appl Phys Lett, 1996, 68(21): 2962-2964. doi: 10.1063/1.116369