基于官能团演化特性的煤氧化动力学研究Kinetic analysis of coal oxidation based on evolution characteristics of functional groups
马腾;陈晓坤;翟小伟;白亚娥;雷昌奎;宋波波;
摘要(Abstract):
为了深入研究煤自燃微观结构的动力学特征,利用同步热分析和原位傅里叶变换红外光谱技术测试顾北烟煤氧化过程中重量与官能团随温度的变化规律。通过Achar微分法与Coast-Redfern积分法相结合对官能团进行动力学计算,并采用Bagchi法推断了最概然机理函数。结果表明:煤氧升温过程呈阶段性变化规律,分为低温失重阶段、吸氧增重阶段、慢化学反应阶段、燃烧阶段和燃尽阶段。煤结构中主要官能团—OH,CO,—CH2,C—H与CC键在各阶段体现出不同氧化特性,在低温失重阶段—OH,—CH2与C—H键参与反应所需要的活化能与遵循动力学模型不同,而CO与CC键结构稳定不易参与反应,从吸氧增重阶段至燃烧阶段,官能团逐渐被激活与氧气发生反应,燃尽阶段官能团基本耗尽。官能团动力学计算结果揭示了煤自燃是各类官能团遵循不同的动力学模型逐步活化的过程。
关键词(KeyWords): 安全科学与工程;煤自燃;动力学;官能团;阶段性
基金项目(Foundation): 国家自然科学基金(51974236)
作者(Author): 马腾;陈晓坤;翟小伟;白亚娥;雷昌奎;宋波波;
Email:
DOI: 10.13800/j.cnki.xakjdxxb.2020.0110
参考文献(References):
- [1] LU Wei,CAO Ying-Jiazi,TIEN Jerry C. Method for prevention and control of spontaneous combustion of coal seam and its application in mining field[J]. International Journal of Mining Science and Technology,2017,27(5):839-846.
- [2] XU Yong-liang,WANG Lan-yun,TIAN Ning,et al.Spontaneous combustion coal parameters for the Crossing-Point Temperature(CPT)method in a Temperature Programmed System(TPS)[J]. Fire Safety Journal,2017,91:147-154.
- [3]张辛亥,白亚娥,李亚清,等.煤升温氧化动力学阶段性规律[J].西安科技大学学报,2017,37(4):474-478.ZHANG Xin-hai,BAI Ya-e,LI Qing-wei,et al. Kinetics and segmentation law of coal oxidation at elevated temperature[J]. Journal of Xi’an University of Science and Technology,2017,37(4):474-478.
- [4]杨漪,邓军,张嬿妮,等.煤氧化特性的STA–FTIR实验研究[J].煤炭学报,2018,43(4):1031-1040.YANG Yi,DENG Jun,ZHANG Yan-ni,et al. Oxidation characteristics of coal by STA-FTIR experiment[J].Journal of China Coal Society,2018,43(4):1031-1040.
- [5]王继仁,邓存宝,单亚飞,等.煤的自燃倾向性新分类方法[J].煤炭学报,2008,33(1):47-50.WANG Ji-ren,DENG Cun-bao,SHAN Ya-fe,et al. A new classifying method of the spontaneous combustion tendency[J]. Journal of China Coal Society,2008,33(1):47-50.
- [6] DENG Jun,REN Li-feng,MA Li,et al. Effect of oxygen concentration on low temperature exothermic oxidation of pulverized coal[J]. Thermochimica Acta,2018,667:102-110.
- [7] Kok MV. Simultaneous thermogravimetry-calorimetry study on the combustion of coal samples:effect of heating rate[J]. Energy Conversion and Management,2012,53:40-4.
- [8]仲晓星,王德明,尹晓丹.基于程序升温的煤自燃临界温度测试方法[J].煤炭学报,2010,35(S1):128-131.ZHONG Xiao-xing,WANG De-ming,YIN Xiao-dan.Test method of critical temperature of coal spontaneous combustion based on the temperature programmed experiment[J]. Journal of China Coal Society,2010,35(S1):128-131.
- [9]邓军,李青蔚,肖旸,等.原煤和氧化煤的低温氧化特性[J].西安科技大学学报,2018,38(1):1-7.DENG Jun,LI Qing-wei,XIAO Yang,et al. Characteristics of low-temperature oxidation of raw and oxidized coals[J]. Journal of Xi’an University of Science and Technology,2018,38(1):1-7.
- [10]屈丽娜,刘星魁,张红元.煤自燃阶段动力学参数及特征温度点的实验研究[J].西安科技大学学报,2015,35(5):597-601.QU Li-na,LIU Xing-kui,ZHANG Hong-yuan. Experimental study of stage characteristic parameters and temperature on coal spontaneous combustion[J]. Journal of Xi’an University of Science and Technology,2015,35(5):597-601.
- [11]王继仁,邓存宝.煤微观结构与组分量质差异自燃理论[J].煤炭学报,2007,32(12):1291-1296.WANG Ji-ren,Deng Cun-bao. The spontaneous combustion theory of coalm icrocosm ic structure and component differences in quantity and quality[J]. Journal of China Coal Society,2007,32(12):1291-1296.
- [12]张国枢,谢应明,顾建明.煤炭自燃微观结构变化的红外光谱分析[J].煤炭学报,2003,28(5):473-476.ZHANG Guo-shu,Xie Ying-ming,Gu Jian-ming. Infrared spectroscopy analysis of microstructure change of coal spontaneous combustion[J]. Journal of China Coal Society,2003,28(5):473-476.
- [13] DENG Jun,YANG Yi,ZHANG Yan-ni,et al. Inhibiting effects of three commercial inhibitors in spontaneous coal combustion[J]. Energy,2018,160:1174-1185.
- [14] DUAN Wen-jun,YU Qing-bo,XIE Hua-qing,et al. Pyrolysis of coal by solid heat carrier-experimental study and kinetic modeling[J]. Energy,2017,135:317-326.
- [15] TIAN Lu-ning,CHEN Han-ping,CHEN Zhen-hui,et al.A study of non-isothermal kinetics of limestone decomposition in air(O2/N2)and oxy-fuel(O2/CO2)atmospheres[J]. Journal of Thermal Analysis and Calorimetry,2014,115(1):45-47.
- [16]肖旸,马砺,王振平,等.采用热重分析法研究煤自燃过程的特征温度[J].煤炭科学技术,2007,35(5):73-76.XIAO Yang,MA Li,WANG Zhen-ping,et al. Research on characteristic temperature in coal spontaneous combustion with thermal gravity analysis method[J]. Coal Science and Technology,2007,35(5):73-76.
- [17] QI Xu-yao,LI Qi-zhong,ZHANG Hui-jun,et al. Thermodynamic characteristics of coal reaction under low oxygen concentration conditions[J]. Journal of the Energy Institute,2017,90(4):544-555.
- [18]许涛.煤自燃过程分段特性及机理的实验研究[D].徐州:中国矿业大学,2012.XU Tao. Experimental study on the subsection characteristic and mechanism of spontaneous combustion of coal[D]. Xuzhou:China University of Mining and Technology,2012.
- [19] QI Xu-yao,WANG De-ming,XIN Hai-hui,et al. In situ FTIR study of real-time changes of active groups during oxygen-free reaction of coal[J]. Energy&Fuels,2013,27(6):3130-3136.
- [20] Walker R,Mastalerz M. Functional group and individual maceral chemistry of high volatile bituminous coals from southern Indiana:controls on coking[J]. Internatioal Journal of Coal Geology,2004,58(3):181-191.
- [21]杨漪.基于氧化特性的煤自燃阻化剂机理及性能研究[D].西安:西安科技大学,2015.YANG Yi,Mechanism and Performance of Inhibitor Based on Oxidation Characteristic of the Spontaneous Combustion of Coal[D]. Xi’an:Xi’an University of Science and Technology,2015.