Numerical simulation of gas solid reaction process in silicon powder nitriding conveying bed

doi:10.16085/j.issn.1000-6613.2021-1191

Abstract

Abstract:

Based on the model of the nucleation reduction of single silicon particles, a mathematical coupling model of reaction, radiation and convection heat transfer of silicon particles in the conveying bed was established. With the help of CFD software FLUENT, the process of energy and mass transfer in the conveying bed was numerically simulated, and the effects of wall temperature, nitrogen flow rate, preheating temperature and particle size of silicon powder, powder gas ratio and diluent ratio on the temperature field and conversion rate of silicon powder in the conveying bed were analyzed. In this paper, a method was proposed to transform the reaction process of single particle into the whole reaction process of particle group in the numerical calculation domain, and the particle size and unreacted silicon particle size can be continuously monitored, which provided a new idea for numerical simulation of granular flow reaction. The reaction process of silicon powder in the conveying bed was similar to that of pulverized coal combustion, and a high temperature zone would be formed in the conveying bed to accelerate the nitriding process of silicon powder. The higher the reaction temperature and the smaller the particle size, the more intense the reaction process and the shorter the time required for the silicon powder to reach complete nitriding. The model showed that in order to make the silicon powder with the particle size of 2.5μm react completely and the maximum temperature did not exceed the decomposition temperature of Si₃N₄ at 2173K, the wall temperature of conveying bed should be controlled at 1773K in the nitridation time of above 170s at the preheating temperature of 1273K with the ratio of powder to gas of 0.2 and the diluent ratio between 0.5 and 1.

Key words: silicon nitride, energy and mass transfer, granular flow, numerical simulation, fluidization, direct nitridation, conveying bed

摘要：

以单个硅颗粒氮化反应缩核模型为基础，本文建立了硅颗粒在输送床内反应、辐射与对流传热耦合的数学模型，并借助CFD软件FLUENT对输送床内能质传输过程进行了数值模拟，分析了输送床壁面温度、氮气流量、预热温度、硅粉粒径等因素对输送床内温度场和硅粉氮化率的影响。在数值计算域内将单个颗粒反应过程转化为颗粒群整体反应过程，实时监测颗粒粒径及未反应硅颗粒粒径，为数值模拟颗粒流反应提供一种新思路。当壁面温度高于1723K时，输送床内会出现一高温区加速硅粉氮化反应；反应温度越高、颗粒粒径越小，氮化过程越剧烈，硅粉到达完全氮化所需时间越短。模型表明为使粒径为2.5μm的硅粉达到完全氮化且输送床内最高温度不超过氮化硅的分解温度2173K，应控制输送床壁面温度在1773K，氮化时间在170s以上，预热温度在1273K，粉气质量比为0.2，稀释剂比例为0.5~1。

关键词: 氮化硅, 能质传输, 颗粒流, 数值模拟, 流态化, 直接氮化, 输送床

CLC Number:

TK124

YIN Shaowu, ZHANG Chao, KANG Peng, HAN Jiawei, WANG Li. Numerical simulation of gas solid reaction process in silicon powder nitriding conveying bed[J]. Chemical Industry and Engineering Progress, 2022, 41(5): 2256-2267.

尹少武, 张朝, 康鹏, 韩嘉维, 王立. 硅粉氮化输送床内气固反应过程数值模拟[J]. 化工进展, 2022, 41(5): 2256-2267.

Figures/Tables 9

References 21

1	肖汉宁, 高朋召. 高性能结构陶瓷及其应用[M]. 北京: 化学工业出版社, 2006: 189.
	XIAO Hanning, GAO Pengzhao. High performance structural ceramics and applications[M]. Beijing: Chemical Industry Press, 2006: 189.
2	RILEY F L. Silicon nitride and related materials[J]. Journal of the American Ceramic Society, 2004, 83(2): 245-265.
3	ZHOU Y, HYUGA H, KUSANO D, et al. Development of high-thermal-conductivity silicon nitride ceramics[J]. Journal of Asian Ceramic Societies, 2015, 3(3): 221-229.
4	GU Y J, LU L L, ZHANG H J, et al. Nitridation of silicon powders catalyzed by cobalt nanoparticles[J]. Journal of the American Ceramic Society, 2015, 98(6): 1762-1768.
5	TOPATEŞ G. Direct production of Si₃N₄ foams by carbothermal reduction and nitridation of SiO₂ [J]. Ceramics International, 2018, 44(16): 20545-20550.
6	YANG J H, HAN L S, CHEN Y X, et al. Effects of pelletization of reactants and diluents on the combustion synthesis of Si₃N₄ powder[J]. Journal of Alloys and Compounds, 2012, 511(1): 81-84.
7	雷超, 李克峰, 王健, 等. LDH催化制备单晶α-Si₃N₄纳米线研究[J]. 化工学报, 2018, 69(10): 4471-4478.
	LEI Chao, LI Kefeng, WANG Jian, et al. Catalytic preparation of α-silicon nitride single-crystalline nanowires by layered double hydroxides[J]. CIESC Journal, 2018, 69(10): 4471-4478.
8	FUKUOKA H, SHIMIZU M, OCHIAI H, et al. Preparation of silicon nitride powder by partially nitriding in a fluidized bed and then completing nitridation in a moving bed: US5232677 A[P]. 1993-08-03.
9	LIU Y D, KIMURA S. Fluidized-bed nitridation of fine silicon powder[J]. Powder Technology, 1999, 106(3): 160-167.
10	王立, 尹少武, 董继昌, 等.基于流态化技术常压连续合成氮化硅粉末的方法: CN1792774[P]. 2006-06-28.
	WANG Li, YIN Shaowu, DONG Jichang, et al. Continuous synthesis method of silicon nitride powder at normal pressure based on fluidization technology: CN1792774[P]. 2006-06-28.
11	尹少武, 王立, 刘传平, 等. 硅粉常压直接氮化制备氮化硅粉的研究[J]. 硅酸盐通报, 2008, 27(2): 230-235.
	YIN Shaowu, WANG Li, LIU Chuanping, et al. The study on the preparation of silicon nitride powders by direct nitridation at normal pressure[J]. Bulletin of the Chinese Ceramic Society, 2008, 27(2): 230-235.
12	YANG F M, WANG L, YIN S W, et al. Experimental study on the entrainment characteristics of ultrafine powder in a fluidized bed with vibrator and agitator[J]. Industrial & Engineering Chemistry Research, 2013, 52(3): 1359-1364.
13	ZHENG X L, YIN S W, DING Y L, et al. Experimental study on high concentration entrainment of ultrafine powder[J]. Powder Technology, 2019, 344(15): 133-139.
14	尹少武, 王立, 孙淑凤, 等. 悬浮床氮化硅合成热过程的实验研究与数值模拟[J]. 北京科技大学学报, 2008, 30(10): 1169-1173, 1193.
	YIN Shaowu, WANG Li, SUN Shufeng, et al. Experiment research and numerical simulation of thermal process in a suspended bed for Si₃N₄ synthesis[J]. Journal of University of Science and Technology Beijing, 2008, 30(10): 1169-1173, 1193.
15	陈锦, 杨晶, 尹少武, 等. 基于CFX软件的氮化硅反应炉内热过程的数值模拟[J]. 北京科技大学学报, 2005, 27(6): 710-715.
	CHEN Jin, YANG Jing, YIN Shaowu, et al. Numerical simulation on thermal process in an Si₃N₄-reaction furnace with CFX[J]. Journal of University of Science and Technology Beijing, 2005, 27(6): 710-715.
16	GIDASPOW D. Multiphase flow and fluidization: continuum and kinetic theory description[M]. New York: Academic Press,1994.
17	张月梅, 黄国强, 苏国良. 导向管喷动流化床内宽筛分硅颗粒流化特性的实验及模拟[J]. 化工进展, 2017, 36(7): 2381-2392.
	ZHANG Yuemei, HUANG Guoqiang, SU Guoliang. Experiment and simulation on the flow characteristics of silicon particles with a wide size distribution in draft tube spout-fluid bed[J]. Chemical Industry and Engineering Progress, 2017, 36(7): 2381-2392.
18	陶文铨. 数值传热学[M]. 2版. 西安: 西安交通大学出版社,2001.
	TAO Wenquan. Numerical heat transfer[M]. 2nd Ed. Xi’an: Xi’an Jiaotong University Press, 2001.
19	金涌. 流态化工程原理[M]. 北京: 清华大学出版社, 2001.
	JIN Yong. Fluidization engineering principles[M]. Beijing: Tsinghua University Press, 2001.
20	JOVANOVIC Z R. Kinetic study on the production of silicon nitride by direct nitridation of silicon in a fluidized bed: experiment and modeling[D]. America: Oregon State University, 1995.
21	段生朝, 麻建军, 郭汉杰, 等. 硅粉直接氮化反应热力学分析及动力学机理研究[J]. 有色金属科学与工程, 2016, 7(4): 14-21.
	DUAN Shengchao, MA Jianjun, GUO Hanjie, et al. Thermodynamic analysis and kinetics mechanism for direct nitridation reaction[J]. Nonferrous Metals Science and Engineering, 2016, 7(4): 14-21.

[1]	GUO Qiang, ZHAO Wenkai, XIAO Yonghou. Numerical simulation of enhancing fluid perturbation to improve separation of dimethyl sulfide/nitrogen via pressure swing adsorption [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 64-72.
[2]	SHAO Boshi, TAN Hongbo. Simulation on the enhancement of cryogenic removal of volatile organic compounds by sawtooth plate [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 84-93.
[3]	WANG Tai, SU Shuo, LI Shengrui, MA Xiaolong, LIU Chuntao. Dynamic behavior of single bubble attached to the solid wall in the AC electric field [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 133-141.
[4]	CHEN Kuangyin, LI Ruilan, TONG Yang, SHEN Jianhua. Structure design of gas diffusion layer in proton exchange membrane fuel cell [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 246-259.
[5]	YANG Yudi, LI Wentao, QIAN Yongkang, HUI Junhong. Analysis of influencing factors of natural gas turbulent diffusion flame length in industrial combustion chamber [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 267-275.
[6]	CHEN Lin, XU Peiyuan, ZHANG Xiaohui, CHEN Jie, XU Zhenjun, CHEN Jiaxiang, MI Xiaoguang, FENG Yongchang, MEI Deqing. Investigation on the LNG mixed refrigerant flow and heat transfer characteristics in coil-wounded heat exchanger (CWHE) system [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4496-4503.
[7]	LIU Xuanlin, WANG Yikai, DAI Suzhou, YIN Yonggao. Analysis and optimization of decomposition reactor based on ammonium carbamate in heat pump [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4522-4530.
[8]	ZHAO Xi, MA Haoran, LI Ping, HUANG Ailing. Simulation analysis and optimization design of mixing performance of staggered impact micromixer [J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4559-4572.
[9]	YE Zhendong, LIU Han, LYU Jing, ZHANG Yaning, LIU Hongzhi. Optimization of thermochemical energy storage reactor based on calcium and magnesium binary salt hydrates [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4307-4314.
[10]	YU Junnan, YU Jianfeng, CHENG Yang, QI Yibo, HUA Chunjian, JIANG Yi. Performance prediction of variable-width microfluidic concentration gradient chips by deep learning [J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3383-3393.
[11]	SHAN Xueying, ZHANG Meng, ZHANG Jiafu, LI Lingyu, SONG Yan, LI Jinchun. Numerical simulation of combustion of flame retardant epoxy resin [J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3413-3419.
[12]	WANG Shuo, ZHANG Yaxin, ZHU Botao. Prediction of erosion life of coal water slurry pipeline based on grey prediction model [J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3431-3442.
[13]	ZHOU Longda, ZHAO Lixin, XU Baorui, ZHANG Shuang, LIU Lin. Advances in electrostatic-cyclonic coupling enhanced multiphase media separation research [J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3443-3456.
[14]	JIN Yong, CHENG Yi, BAI Dingrong, ZHANG Chenxi, WEI Fei. Fluidization research and development in China [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2761-2780.
[15]	ZHANG Kai, JIN Hanyu, LIU Siyu, WANG Shuai. Simulation of mass transfer process under the bubble interaction in bubbling fluidization [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2828-2835.