Effect of raw material size on the synthesis of silicon carbide

doi:10.11949/0438-1157.20200981

Abstract

Abstract:

Using tire semi-coke as carbon source and silicon sand as silicon source,silicon carbide(SiC) was prepared by carbothermal reduction method at 1520℃. XRD, SEM and FTIR spectrometer were used to characterize the SiC prepared under different raw material particle size conditions. The influence law of raw material particle size on the phase, morphology, particle size and reaction degree of the synthesized SiC was investigated. The results show that the size of the raw material has a very important influence on the degree of synthesis reaction and the phase composition, morphology and size of the product.Within a certain particle size range, with the decrease of silicon sand particle size, SiC crystal type becomes complete and SiC whisker decreases gradually, while the SiC particle size distribution does not change significantly.With the increase of semi-coke size of tire, the product phase gradually becomes single, and the proportion of SiC particle size and whisker decreases gradually. In addition, by measuring the C/Si ratio in the product and confirming the presence of the intermediate product SiO, it is inferred that the formation mechanism of SiC particles is gas-solid (VS) reaction, while the formation mechanism of SiC whiskers is gas-gas(VV) reaction.

Key words: tire carbocoal, SiC, particle size distribution, carbothermic reduction, generation mechanism

摘要：

以轮胎半焦为碳源，石英砂为硅源，在1520℃下通过碳热还原法制备了碳化硅。采用XRD、SEM和红外光谱仪等对不同原料粒度条件下制备的碳化硅进行了表征，探究了原料粒度对合成碳化硅物相、形貌、粒度和反应程度的影响规律。结果表明：原料粒度对碳化硅的合成反应进行程度及产物碳化硅的物相组成、形貌、粒度均有十分重要的影响。在一定粒度范围内，随着石英砂粒度的减小，碳化硅晶型变完整，且晶须逐渐减少，碳化硅的粒径分布没有明显变化；随着轮胎半焦粒度的增大，产物物相逐渐变为单一，碳化硅的粒径和晶须所占的比例逐渐减小。此外，通过对产物中C/Si 比的测定和存在中间产物SiO的证实，推测出了碳化硅颗粒的生成机理为气-固（VS）反应，而碳化硅晶须的生成机理为气-气（VV）反应。

关键词: 轮胎半焦, 碳化硅, 粒度分布, 碳热还原, 生成机理

CLC Number:

TB 321

LU Pengfei, JIN Zhihao, CUI Yanbin, XU Guangwen, WU Rongcheng. Effect of raw material size on the synthesis of silicon carbide[J]. CIESC Journal, 2021, 72(4): 2300-2308.

陆鹏飞, 金志浩, 崔彦斌, 许光文, 武荣成. 原料粒度对合成碳化硅的影响研究[J]. 化工学报, 2021, 72(4): 2300-2308.

Figures/Tables 12

Fig.1 SEM image of tire semi-coke

Table 1 Industrial analysis results and elemental analysis of tire semi-coke

Proximate analysis w_ar/%

BET/

(m2/g)

Ultimate analysis w_ar/%

Table 2 Results of chemical analysis of silicon sand

Compositin	Content w_d/%
SiO₂	99.54
CaO	0.06
Fe₂O₃	0.13
Al₂O₃	0.11
MgO	0.08
burn reduces	0.08

Fig.2 Flow chart for SiC preparation

Fig.3 XRD patterns of SiC synthesized by raw materials with different particle sizes

Table 3 The burning loss rate and yield of silicon sand samples with different particle size

Silica sand size/mesh	Reaction loss rate, w_tf/%	Reaction loss rate, w_mf/%	Productive rate, w/%
20—40	28.31	40.48	52.33
50—80	66.99	0.58	91.05
100—120	65.03	2.41	86.41
140—160	63.05	7.53	81.65

Fig.4 SEM images of SiC synthesized by raw materials with different particle size

Fig.5 SiC particle size and size distribution of raw materials with different particle size

Fig.6 SEM images of SiC synthesized by raw materials with different particle size

Table 4 Average particle size of SiC prepared from raw materials with different particle size

Materials	Raw material particle size/mesh	Average particle size of SiC/μm
tire semi-coke	20—35	161.8
	140—160	53.353
	270—325	42.106
silica sand	50—80	37.679
	100—120	40.015
	140—160	38.473

Fig.7 FT-IR spectra of the white substance in the product and SiO

Fig.8 EDS of prepared SiC

References 36

1	Chiew Y L, Cheong K Y. A review on the synthesis of SiC from plant-based biomasses[J]. Materials Science and Engineering: B, 2011, 176(13): 951-964.
2	Siergiej R R, Clarke R C, Sriram S, et al. Advances in SiC materials and devices: an industrial point of view[J]. Materials Science and Engineering: B, 1999, 61/62: 9-17.
3	李冬燕, 魏巍, 韩峰. 高温除尘碳化硅膜的制备及其抗腐蚀特性[J]. 化工学报, 2019, 70(1): 336-344.
	Li D Y, Wei W, Han F. Preparation and corrosion resistance of SiC membrane using for dust removal in high temperature[J]. CIESC Journal, 2019, 70(1): 336-344.
4	Fu Q G, Li H J, Shi X H, et al. Synthesis of silicon carbide nanowires by CVD without using a metallic catalyst[J]. Materials Chemistry and Physics, 2005, 100(1): 108-111.
5	Guo X Y, Jin G Q. Pore-size control in the sol-gel synthesis of mesoporous silicon carbide[J]. Journal of Materials Science, 2005, 40(5): 1301-1303.
6	Yang W, Araki H, Thaveethavorn S, et al. In situ synthesis and characterization of pure SiC nanowires on silicon wafer[J]. Applied Surface Science, 2005, 241(1/2): 236-240.
7	刘巧钰, 李洪, 高鑫, 等. 泡沫碳化硅波纹规整填料内的液体流动特性[J]. 化工学报, 2016, 67(8): 3340-3346.
	Liu Q Y, Li H, Gao X, et al. Liquid flow characteristics of structured corrugation SiC-foam packing sheets[J]. CIESC Journal, 2016, 67(8): 3340-3346.
8	Najafi A, Fard F G, Rezaie H R, et al. Synthesis and characterization of SiC nano powder with low residual carbon processed by sol-gel method[J]. Powder Technology, 2012, 219: 202-210.
9	Lao X B, Xu X Y, Jiang W H, et al. Effect of SiC nanoparticles on in-situ synthesis of SiC whiskers in corundum-mullite-SiC composites obtained by carbothermal reduction[J]. Ceramics International, 2020, 46(7): 9225-9232.
10	Kuang J L, Xiao T, Hou X J, et al. Microwave synthesis of worm-like SiC nanowires for thin electromagnetic wave absorbing materials[J]. Ceramics International, 2019, 45(9): 11660-11667.
11	Shahedi A M, Ahmadi Z, Sabahi N A, et al. Spark plasma sintering of TiC-SiCw ceramics[J]. Ceramics International, 2019, 45(16): 19808-19821.
12	Chen J P, Song G, Liu Z, et al. Preparation of SiC whiskers using graphene and rice husk ash and its photocatalytic property[J]. Journal of Alloys and Compounds, 2020, 833: 155072.
13	Singh D, Zhu D M, Zhou Y C, et al. Design, Development, and Applications of Engineering Ceramics and Composites[M]. John Wiley & Sons, Inc., 2010.
14	Narisawa M, Yasuda H, Mori R, et al. Silicon carbide particle formation from carbon black-polymethylsilsesquioxane mixtures with melt pressing[J]. Journal of the Ceramic Society of Japan, 2008, 116(1349): 121-125.
15	Cui X L, Wang Y H, Wang L, et al. Synthesis of nanometer-sized TiC and SiC from petroleum coke by reactive milling[J]. Petroleum Science and Technology, 2001, 19(7/8): 971-978.
16	Sulardjaka, Jamasri, Wildan M W, et al. Method for increasing β-SiC yield on solid state reaction of coal fly ash and activated carbon powder[J]. Bulletin of Materials Science, 2011, 34(4): 1013-1016.
17	Wang L, Hu X B, Xu X G, et al. Synthesis of high purity SiC powder for high-resistivity SiC single crystals growth[J]. Journal of Materials Science & Technology, 2007, 23(1): 120-124.
18	Guo X Z, Zhu L, Li W Y, et al. Preparation of SiC powders by carbothermal reduction with bamboo charcoal as renewable carbon source[J]. Journal of Advanced Ceramics, 2013, 2(2): 128-134.
19	Liu M, Zeng X, Ma C, et al. Injectable hydrogels for cartilage and bone tissue engineering[J]. Bone Research, 2017, 5: 17014.
20	Shen Z Z, Chen J H, Li B, et al. A novel two-stage synthesis for 3C-SiC nanowires by carbothermic reduction and their photoluminescence properties[J]. Journal of Materials Science, 2019, 54(19): 12450-12462.
21	Wei J, Li K Z, Li H J, et al. Growth and morphology of one-dimensional SiC nanostructures without catalyst assistant[J]. Materials Chemistry and Physics, 2006, 95(1): 140-144.
22	阳永荣, 王靖岱, 颜丽红. 废轮胎热解再生炭黑表面活性[J]. 化工学报, 2005, 56(4): 726-732.
	Yang Y R, Wang J D, Yan L H. Surface character of pyrolytic carbon black[J]. Journal of Chemical Industry and Engineering (China), 2005, 56(4): 726-732.
23	Wang J K, Zhang Y Z, Li J Y, et al. Catalytic effect of cobalt on microwave synthesis of β-SiC powder[J]. Powder Technology, 2017, 317: 209-215.
24	Lin Y J, Tsang C P. The effects of starting precursors on the carbothermal synthesis of SiC powders[J]. Ceramics International, 2003, 29(1): 69-75.
25	Jiang S N, Gao S B, Liu Y, et al. An efficient way of recycling silicon kerf waste for synthesis of high-quality SiC[J]. International Journal of Applied Ceramic Technology, 2020, 17(1): 130-137.
26	Guo X Z, Zhang L J, Yan L Q, et al. Preparation of silicon carbide using bamboo charcoal as carbon source[J]. Materials Letters, 2009, 64(3): 331-333.
27	An Z B, Xue J, Cao H, et al. A facile synthesis of silicon carbide nanoparticles with high specific surface area by using corn cob[J]. Advanced Powder Technology, 2018, 30(1): 164-169.
28	古卫俊, 贾素秋, 邱敬东, 等. 稻壳制备碳化硅晶须[J]. 硅酸盐学报, 2014, 42(1): 28-32.
	Gu W J, Jia S Q, Qiu J D, et al. Preparation of SiC whiskers from rice husk[J]. Journal of the Chinese Ceramic Society, 2014, 42(1): 28-32.
29	郝建英, 王英勇, 童希立, 等. 不同碳硅比对合成高比表面积炭化硅的影响[J]. 材料导报, 2012, 26(10): 73-76.
	Hao J Y, Wang Y Y, Tong X L, et al. Effect of n(C)/n(Si) on the synthesis of high surface area SiC[J]. Materials Review, 2012, 26(10): 73-76.
30	蒙真真, 武志红, 刘新伟, 等. 竹节状碳化硅晶须吸波性能研究[J]. 化工学报, 2020, 71(4): 1889-1897.
	Meng Z Z, Wu Z H, Liu X W, et al. Study on absorbing properties of bamboo-like silicon carbide whiskers[J]. CIESC Journal, 2020, 71(4): 1889-1897.
31	Park W S, Joo B J, Choi D J, et al. A study on the thermal stability of silicon carbide whiskers on growth temperature[J]. Journal of Materials Science, 2005, 40(20): 5529-5531.
32	Silva P C, Figueiredo J L. Production of SiC and Si₃N₄ whiskers in C+SiO₂ solid mixtures[J]. Materials Chemistry and Physics, 2001, 72(3): 326-331.
33	Li X K, Liu L, Zhang Y X, et al. Synthesis of nanometre silicon carbide whiskers from binary carbonaceous silica aerogels[J]. Carbon, 2001, 39(2): 159-165.
34	Niu F X, Wang Y X, Fu S L, et al. Ferrocene-assisted growth of SiC whiskers with hexagonal cross-section from a preceramic polymer[J]. Ceramics International, 2017, 43(15): 12983-12987.
35	杨书廷, 杨伟光, 尹艳红, 等. 微波热处理对La-Ni-Pt纳米合金催化剂性质的影响[J]. 材料热处理学报, 2006, 27(5): 22-25, 131.
	Yang S T, Yang W G, Yin Y H, et al. Influence of microwave heat-treatment on properties of La-Ni-Pt nano-alloy catalysts[J]. Transactions of Materials and Heat Treatment, 2006, 27(5): 22-25, 131.
36	Choi H J, Lee J G. Stacking faults in silicon carbide whiskers[J]. Ceramics International, 2000, 26(1): 7-12.

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