气相爆轰合成碳包铁的影响因素

doi:10.15541/jim20150544

无机材料学报 ›› 2016, Vol. 31 ›› Issue (5): 542-546.DOI: 10.15541/jim20150544

气相爆轰合成碳包铁的影响因素

闫鸿浩1, 赵铁军1, 孙贵磊3, 李晓杰1,2, 浑长宏1

(1. 大连理工大学工程力学系, 大连116024; 2. 大连理工大学工业装备结构分析国家重点实验室, 大连 116024; 3. 中国劳动关系学院安全工程系, 北京 100048)

收稿日期:2015-11-09 修回日期:2015-12-12 出版日期:2016-05-20 网络出版日期:2016-04-25
作者简介:闫鸿浩(1974–), 男, 博士, 副研究员. E-mail: honghaoyan@vip.sina.com
基金资助:
国家自然科学基金(10872044, 10602013, 10972051, 10902023).辽宁省自然科学基金(20082161), 北京高等学校

Influence Factors of Preparing Carbon-encapsulated Iron Nanoparticles by Gaseous Detonation Method

YAN Hong-Hao¹, ZHAO Tie-Jun¹, SUN Gui-Lei³, LI Xiao-Jie^1,2, HUN Chang-Hong¹

(1. Department of Engineering Mechanics, Dalian University of Technology, Dalian 116024, China; 2. State Key Laboratory of Structural Analysis for Industrial Equipment, Dalian 116024, China; 3. Department of Safety Engineering, China Institute of Industrial Relations, Beijing, 100048, China)

Received:2015-11-09 Revised:2015-12-12 Published:2016-05-20 Online:2016-04-25
About author:YAN Hong-Hao. E-mail: honghaoyan@vip.sina.com
Supported by:
National Natural Science Foundation of China (10872044, 10602013, 10972051, 10902023).Natural Science Foundation

摘要/Abstract

摘要：

研究了氢氧摩尔比例与二茂铁质量对制备碳包覆铁纳米颗粒的影响。通过氢气与氧气爆轰产生的高温高速, 在自制爆轰管内分解二茂铁, 合成了碳包覆铁纳米颗粒。经XRD分析与TEM表征发现, 氢氧比例与二茂铁质量在制备碳包铁时相互影响, 氢氧比例主要影响碳包铁的形貌大小及分散性, 二茂铁质量对能否合成碳包铁纳米颗粒影响很大。当氢氧比例为2:1, 二茂铁质量在2.5~3.5 g时, 能够合成碳包覆铁纳米颗粒, 且呈球形或椭球形, 具有明显的核壳结构。从颗粒大小均匀性, 形貌结构及分散性考虑, 氢氧比例2:1, 二茂铁质量3.5 g的反应条件是制备碳包铁的较佳方案。

关键词: 气相爆轰法, 碳包铁, 氢氧比例, 二茂铁

Abstract:

Effects of molar ratio of hydrogen to oxygen and ferrocene mass on synthesis of carbon-encapsulated iron nanoparticles (Fe@C) were studied. Fe@C were prepared by using ferrocene as material resource, which decomposed by high temperature and high speed caused by hydrogen and oxygen detonation in homemade detonation tube. The samples were characterized by X-ray diffraction, transmission electron microscope and high resolution transmission electron microscope and it can be found that the molar ratio of hydrogen to oxygen, and ferrocene mass interact each other in the preparation of Fe@C. The molar ratio of hydrogen to oxygen mainly influences the morphology, particle size and dispersion of Fe@C, while ferrocene mass has a great affect on the synthesis of Fe@C. Part of iron element will be oxidized at small dosage of ferrocene, on the contrary, ferrocene couldn’t be decomposed completely. When the molar ratio of hydrogen to oxygen is 2:1, ferrocene mass ranges in 2.5-3.5 g, spherical or ellipsoidal like Fe@C is prepared with a clear core-shell structure, and thickness of carbon shell at about 10 nm. In consideration of particle size uniformity, morphology structure and dispersion, the best condition for preparing Fe@C is, the molar ratio of hydrogen to oxygen at 2:1, ferrocene mass at 3.5 g.

Key words: gaseous detonation method, carbon-encapsulated iron, hydrogen and oxygen ratio, ferrocene

中图分类号:

O389

闫鸿浩, 赵铁军, 孙贵磊, 李晓杰, 浑长宏. 气相爆轰合成碳包铁的影响因素[J]. 无机材料学报, 2016, 31(5): 542-546.

YAN Hong-Hao, ZHAO Tie-Jun, SUN Gui-Lei, LI Xiao-Jie, HUN Chang-Hong. Influence Factors of Preparing Carbon-encapsulated Iron Nanoparticles by Gaseous Detonation Method[J]. Journal of Inorganic Materials, 2016, 31(5): 542-546.

图/表 12

图1 气相爆轰管的示意图

Fig. 1 Schematic of gaseous detonation tube

表1 不同氢氧比例的实验初始条件

Table 1 Conditions of initial experimental with different ratio of hydrogen to oxygen

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	140	0.1	3.5	1:1
2#	140	0.1	3.5	2:1

表2 不同二茂铁质量的实验初始条件

Table 2 Conditions of initial experimental with different ferrocene mass

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

表3 反应物中各元素的摩尔构成及其氧平衡

Table 3 Moles of each element in the reactants and the corresponding oxygen balance

Sample	Mole of each element				n(H):n(O)	Oxygen balance
Sample	H	O	C	Fe	n(H):n(O)	Oxygen balance
1#	0.536	0.348	0.188	0.0188	1.5:1.0	<0
2#	0.652	0.232	0.188	0.0188	2.8:1.0	<0

图2 不同氢氧比例制备样品的XRD图谱

Fig. 2 XRD patterns of samples prepared with different ratio of hydrogen to oxygen

表4 爆轰产物的平均粒径

Table 4 Average particle size of the detonation products

Sample	Phases	2θ/(°)	FWHM	Mean grain size, D/nm
1#	Fe	44.5	0.274	31
1#	Fe₃C	43.2	0.401	21
2#	Fe	44.5	0.374	23
2#	Fe₃C	43.3	0.553	16

图3 不同氢氧比例制备样品的TEM照片

Fig. 3 TEM images of samples prepared with different ratio of hydrogen to oxygen Ratios of hydrogen to oxygen of A to B are 1:1, 2:1, respectively

表5 反应物中各元素的摩尔构成及其氧平衡

Table 5 Moles of each element in the reactants and the corresponding oxygen balance

Sample	Mole of each element				n(H):n(O)	Oxygen balance
Sample	H	O	C	Fe	n(H):n(O)	Oxygen balance
1#	0.545	0.232	0.081	0.0081	2.3:1	<0
2#	0.598	0.232	0.134	0.0134	2.6:1	<0
3#	0.625	0.232	0.161	0.0161	2.7:1	<0
4#	0.652	0.232	0.188	0.0188	2.8:1	<0
5#	0.679	0.232	0.215	0.0215	2.9:1	<0

图4 不同二茂铁质量合成产物的XRD图谱

Fig. 4 XRD patterns of detonation products with different ferrocene mass Ferrocene mass of 1#, 2#, 3#, 4# and 5# are 1.5, 2.5, 3.0, 3.5 and 4.0 g, respectively

表6 爆轰产物中铁颗粒的平均粒径

Table 6 Average particle size of iron in detonation products

Sample	Phases	2θ/(°)	FWHM	Mean grain size, D/nm
1#	Fe	44.5	0.169	50
2#	Fe	44.6	0.275	30
3#	Fe	44.6	0.221	38
4#	Fe	44.5	0.374	23
5#	Fe	44.6	0.264	32

图5 不同二茂铁质量获得产物的TEM照片

Fig. 5 TEM images of detonation products with different ferrocene masses Ferrocene mass: A) 1.5 g; B) 2.5 g; C) 3.5 g

图6 不同二茂铁质量制备产物的HR-TEM照片

Fig. 6 HR-TEM images of detonation products prepared with different ferrocene masses Ferrocene mass: (a) 1.5 g; (b) 2.5 g; (c) 3.5 g

参考文献 13

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气相爆轰合成碳包铁的影响因素

Influence Factors of Preparing Carbon-encapsulated Iron Nanoparticles by Gaseous Detonation Method

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Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

[1]	郑国斌,施益峰,冯景伟,郭景坤. 流动催化法连续制备碳纳米管及其形态和结构的研究[J]. 无机材料学报, 2001, 16(5): 945-950.
[2]	张海燕,何艳阳,薛新民,成晓玲,彭少麒. 碳弧法中碳包Fe纳米晶及其相关碳微团的形成[J]. 无机材料学报, 1999, 14(2): 291-296.

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1

Sample	Temperature/℃	Initial pressure/MPa	Ferrocene mass/g	n(H₂):n(O₂)
1#	120	0.1	1.5	2:1
2#	120	0.1	2.5	2:1
3#	120	0.1	3.0	2:1
4#	120	0.1	3.5	2:1
5#	120	0.1	4.0	2:1