基于阻抗特征煤体中瓦斯因素对水合动力学的影响
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摘要
为研究不同瓦斯赋存条件下水合机理防治煤与瓦斯突出的基础规律,利用阻抗特性监测与高压瓦斯水合实验一体化装置,针对4种瓦斯气体分别在4种赋存压力(4 MPa,5 MPa,6 MPa,7 MPa)条件下开展煤体中瓦斯水合实验,根据阻抗特征获取了瓦斯水合物形成诱导时间,计算了煤体中瓦斯水合物生长速率与饱和度。结果表明:煤体中瓦斯水合过程中上层位与中层位阻抗逐渐增大,下层位阻抗逐渐减小,瓦斯水合物主要分布于上层位与中层位煤体中;随初始压力变化瓦斯水合物形成诱导时间未呈现规律性变化,随着混合气中CH_4浓度的下降,诱导时间先减小后增大,实验范围内平均诱导时间为41 min,分布范围为18～74 min;随初始压力与瓦斯气体组分浓度的变化煤体中瓦斯水合物平均生长速率呈振荡变化趋势,平均生长速率均值为0.58 cm~3·min~(-1),最快为0.84 cm~3·min~(-1);煤体中瓦斯水合物的饱和度随初始压力与瓦斯中CH_4浓度的增大呈逐渐升高的变化趋势,水合物饱和度范围为17.03%～57.03%。
The goal of this research was to study the basic law of hydration mechanism to prevent coal and gas outburst under different gas occurrence conditions. Impedance characteristic monitoring and high pressure gas hydrate experimental device is used to carry out gas hydration experiment in coal on condition of 4 kinds of mine gas in different occurrence pressure which are 4 MPa, 5 MPa, 6 MPa and 7 MPa respectively. The induction time of gas hydrate formation is obtained according to the impedance characteristics. Meanwhile, the growth rate and saturation of mine gas hydrate are calculated. The results show that impedance value increases in the upper layer and it decreases in the lower layer in the process of mine gas hydration in coal, which also indicates that mine gas hydrate mainly forms in the upper and middle layer of the experimental reactor. The induction time of gas hydrate formation does not change regularly with the different initial pressure. However, with the decrease of CH4 concentration in the mixture gas, the induction time declines at the beginning and then rises up. The average induction time is 41 min with the range from 18 min to 74 min. The average growth rate of the gas hydrate in the coal displays the oscillation tendency with the change of initial pressure and the gas component concentration. The average growth rate is 0.58 cm~3·min~(-1) and the fastest is up to 0.84 cm~3·min~(-1). The saturation of mine gas hydrate rises gradually with the increase of initial pressure and CH4 concentration in mine gas in which the saturation ranges from 17.03% to 57.03%.
The goal of this research was to study the basic law of hydration mechanism to prevent coal and gas outburst under different gas occurrence conditions. Impedance characteristic monitoring and high pressure gas hydrate experimental device is used to carry out gas hydration experiment in coal on condition of 4 kinds of mine gas in different occurrence pressure which are 4 MPa, 5 MPa, 6 MPa and 7 MPa respectively. The induction time of gas hydrate formation is obtained according to the impedance characteristics. Meanwhile, the growth rate and saturation of mine gas hydrate are calculated. The results show that impedance value increases in the upper layer and it decreases in the lower layer in the process of mine gas hydration in coal, which also indicates that mine gas hydrate mainly forms in the upper and middle layer of the experimental reactor. The induction time of gas hydrate formation does not change regularly with the different initial pressure. However, with the decrease of CH4 concentration in the mixture gas, the induction time declines at the beginning and then rises up. The average induction time is 41 min with the range from 18 min to 74 min. The average growth rate of the gas hydrate in the coal displays the oscillation tendency with the change of initial pressure and the gas component concentration. The average growth rate is 0.58 cm~3·min~(-1) and the fastest is up to 0.84 cm~3·min~(-1). The saturation of mine gas hydrate rises gradually with the increase of initial pressure and CH4 concentration in mine gas in which the saturation ranges from 17.03% to 57.03%.
引文
[1]贾宝山,李春苗,尹彬,等.基于CHEMKIN-PRO的多元混合气体瓦斯燃烧模拟研究[J].煤炭学报,2017, 42(3):646-652JIA Baoshan, LI Chunmiao, YIN Bin, et al. Computing Study on Multivariate Mixed Gas Burning by CHEMKINPRO Software[J]. Journal of China Coal Society. 2017,42(03):646-652
[2]张强,吴强,张保勇,等.阻抗测试方法在瓦斯水合防突模拟实验中的应用[J].煤炭学报,2016, 41(12):3047-3053ZHANG Qiang, WU Qiang, ZHANG Baoyong, et al. Application of Impedance Test Method in the Simulation Experiment of Mine Gas Hydrate Outburst Prevention[J].Journal of China Coal Society, 2016, 41(12):3047-3053
[3] SLOAN E D, KOH C A. Clathrate Hydrates of Natural Gases[M].3rd ed. Boca Raton:CRC Press, 2008:10-20
[4]高霞,刘文新,高橙,等.含瓦斯水合物煤体强度特性三轴试验研究[J].煤炭学报,2015, 40(12):2829-2835GAO Xia, LIU Wenxin, GAO Chen, et al. Triaxial Shear Strength of Methane Hydrate-bearing Coal[J]. Journal of China Coal Society, 2015, 40(12):2829-2835
[5]吴强,朱福良,高霞,等.晶体类型对含瓦斯水合物煤体力学性质的影响[J].煤炭学报,2014, 39(8):1492-1496WU Qiang, ZHU Fuliang, GAO Xia, et al. Effect of Hydrate Crystal Type on Mechanical Properties of Gas Hydrate-bearing Coal[J]. Journal of China Coal Society,2014, 39(8):1492-1496
[6]吴强,张保勇.瓦斯水合物在含煤表面活性剂溶液中生成影响因素[J].北京科技大学学报,2007, 29(08):755-758+770WU Qiang, ZHANG Baoyong. Influence Factors of Mine Gas Hydrate Formation in Surfactant Solution Containing Coal[J]. Journal of University of Science and Technology Beijing, 2007, 29(8):755-758+770.
[7]吴强,李成林,江传力.瓦斯水合物生成控制因素探讨[J].煤炭学报,2005, 30(3):283-287WU Qiang, LI Chenglin, JIANG Chuanli. Discussion on the Control Factors of Forming Gas Hydrate[J]. Journal of China Coal Society, 2005, 30(3):283-287
[8] WU Q, ZHANG Q, ZHANG B Y. Influence of SuperAbsorbent Polymer on the Growth Rate of Gas Hydrate[J]. Safety Science, 2012, 50(4):865-869
[9]张强,吴强,张保勇.NaCl-SDS复合溶液中多组分瓦斯水合物成核动力学机理[J].煤炭学报,2015, 40(10):2430-2436ZHANG Qiang, WU Qiang, ZHANG Baoyong. Nucleation Kinetics Mechanism of Multi-component Mine Gas Hydrate in NaCl-SDS Mixed Solutions[J]. Journal of China Coal Society, 2015, 40(10):2430-2436
[10]吴强,张保勇,王永敬.瓦斯水合物分解热力学研究[J].中国矿业大学学报,2006, 35(5):658-661WU Qiang, ZHANG Baoyong, WANG Yongjing. Study of Decomposition Thermody Namics of Gas Hydrate[J].Journal of China University of Mining&Technology,2006, 35(5):658-661
[11]吴琼,吴强,张保勇,等.丙烷对瓦斯混合气水合物相平衡的影响[J].煤炭学报,2014, 39(7):1283-1288WU Qiong, WU Qiang, ZHANG Baoyong, et al. Effect of Propane on the Phase Equilibrium of Mixture Gas Hydrate[J]. Journal of China Coal Society, 2014, 39(7):1283-1288
[12] SURYA D, ALEXANDER G, ALLAN S M. THF-water Hydrate Crystallization:an Experimental Investigation[J]. Journal of Crystal Growth, 1999, 204(4):525-538
[13] SHARMA D, SOWJANYA Y, DHANUNJANA C V, et al. Methane Storage in Mixed Hydrates with Tetrahydrofuran[J].Indian of Chemical Technology, 2014, 21(21):114-119
[14] SHENG D, JOO Y L, CARLOS S. Hydrate Nucleation in Quiescent and Dynamic Conditions[J]. Fluid Phase Equilibria, 2014, 378:107-112
[15]叶楠.季盐类水合物相平衡条件及生长动力学研究[D].上海:上海交通大学,2014YE Nan. Equilibrium Conditions and Kinetics of Hydrates Forming with Quaternary Salts[D]. Shanghai:Shanghai Jiao Tong University, 2014
[16]许浪.瓦斯爆炸冲击波衰减规律及安全距离研究[D].徐州:中国矿业大学,2015XU Lang. Study on Phase Equilibrium Theoretical Predictions and Dynamic Characteristics of gas Hydrate in the Complex System Containing Thermodynamic Additives[D]. Xuzhou:China University of Mining and Technology, 2015
[17]孙国庆.THF和TBAB对煤层气水合物相平衡影响的实验及理论研究[D].太原:太原理工大学,2015SUN Guoqing. Experimental and Theoretical Research of the Effect of TBAB and THF on Coal-bed Methane Hydrate Phase Equilibrium[D]. Taiyuan:Taiyuan University of Technology, 2015
[18]周诗岽,余益松,王树立,等.管道流动体系下天然气水合物生成模型的研究进展[J].天然气工业,2014, 34(2):92-98ZHOU Shidong, YU Yisong, WANG Shuli, et al.Rescearch Progress in the Natural Gas Hydrate Formation Model Under the Pipe Flow System[J]. Natural Gas Industry, 2014, 34(2):92-98
[19]赵欣,邱正松,江琳,等.动力学抑制剂作用下天然气水合物生成过程的实验分析[J].天然气工业,2014, 34(2):105-110ZHAO Xin, QIU Zhengsong, JIANG Lin, et al. An Experimental Analysis of Natural Gas Hydrate Formationat the Presence of Kinetic Hydrate Inhibitors[J]. Natural Gas Industry, 2014, 34(2):105-110
[20]梁德青,臧小亚,吴能友.介观孔隙中天然气水合物生成过程模拟[J].天然气工业,2013, 33(7):24-28LIANG Deqing, ZANG Xiaoya, WU Nengyou. A Simulation Study of Natural Gas Hydrate Generation in Mesoscopic-scale Pores[J]. Natural Gas Industry, 2013,33(7):24-28
[21]金学彬,陈强,邢兰昌,等.多孔介质中甲烷水合物聚散过程的交流阻抗谱响应特征[J].天然气工业,2016, 36(3):120-127JIN Xuebin, CHEN Qiang, XING Lanchang, et al. Response Characteristics of AC Impedance Spectroscopy During the Formation and Dissociation of Methane Hydrate in Porous Media[J]. Natural Gas Industry, 2016,36(3):120-127
[22]任静雅,鲁晓兵,张旭辉.水合物沉积物电阻特性研究初探[J].岩土工程学报,2013, 35(1):161-165REN Jingya, LU Xiaobing, ZHANG Xuhui. Preliminary Study on Electric Resistance of Hydrate-bearing Sediments[J]. Chinese Journal of Geotechnical Engineering,2013, 35(1):161-165
[23] ZATSEPINA O Y, BUFFETT B A. Nucleation of CO_2-hydrate in a Porous Medium[J]. Fluid Phase Equilibria,2002, 200(2):263-275
[24] SLOAN E D, FFLEYFEL J R. A Molecular Mechanism for Gas Hydrate Nucleation From Ice[J]. AIChE Journal,1991, 37(9):146-151
[25] CHRISTIANSEN R L, SLOAN E D. Mechanisms and Kinetics of Hydrate Formation[J]. Annals of the New York Academy of Sciences, 1994, 715(1):283-305
[26]陈光进,孙长宇,马庆兰.气体水合物科学与技术[M].北京:化学工业出版社,2007CHEN Guangjin, SUN Changyu, MA Qinglan. Scientific and Technology of Gas Hydrate[M]. Beijing:Chemical Industry Publishing House, 2007
[2]张强,吴强,张保勇,等.阻抗测试方法在瓦斯水合防突模拟实验中的应用[J].煤炭学报,2016, 41(12):3047-3053ZHANG Qiang, WU Qiang, ZHANG Baoyong, et al. Application of Impedance Test Method in the Simulation Experiment of Mine Gas Hydrate Outburst Prevention[J].Journal of China Coal Society, 2016, 41(12):3047-3053
[3] SLOAN E D, KOH C A. Clathrate Hydrates of Natural Gases[M].3rd ed. Boca Raton:CRC Press, 2008:10-20
[4]高霞,刘文新,高橙,等.含瓦斯水合物煤体强度特性三轴试验研究[J].煤炭学报,2015, 40(12):2829-2835GAO Xia, LIU Wenxin, GAO Chen, et al. Triaxial Shear Strength of Methane Hydrate-bearing Coal[J]. Journal of China Coal Society, 2015, 40(12):2829-2835
[5]吴强,朱福良,高霞,等.晶体类型对含瓦斯水合物煤体力学性质的影响[J].煤炭学报,2014, 39(8):1492-1496WU Qiang, ZHU Fuliang, GAO Xia, et al. Effect of Hydrate Crystal Type on Mechanical Properties of Gas Hydrate-bearing Coal[J]. Journal of China Coal Society,2014, 39(8):1492-1496
[6]吴强,张保勇.瓦斯水合物在含煤表面活性剂溶液中生成影响因素[J].北京科技大学学报,2007, 29(08):755-758+770WU Qiang, ZHANG Baoyong. Influence Factors of Mine Gas Hydrate Formation in Surfactant Solution Containing Coal[J]. Journal of University of Science and Technology Beijing, 2007, 29(8):755-758+770.
[7]吴强,李成林,江传力.瓦斯水合物生成控制因素探讨[J].煤炭学报,2005, 30(3):283-287WU Qiang, LI Chenglin, JIANG Chuanli. Discussion on the Control Factors of Forming Gas Hydrate[J]. Journal of China Coal Society, 2005, 30(3):283-287
[8] WU Q, ZHANG Q, ZHANG B Y. Influence of SuperAbsorbent Polymer on the Growth Rate of Gas Hydrate[J]. Safety Science, 2012, 50(4):865-869
[9]张强,吴强,张保勇.NaCl-SDS复合溶液中多组分瓦斯水合物成核动力学机理[J].煤炭学报,2015, 40(10):2430-2436ZHANG Qiang, WU Qiang, ZHANG Baoyong. Nucleation Kinetics Mechanism of Multi-component Mine Gas Hydrate in NaCl-SDS Mixed Solutions[J]. Journal of China Coal Society, 2015, 40(10):2430-2436
[10]吴强,张保勇,王永敬.瓦斯水合物分解热力学研究[J].中国矿业大学学报,2006, 35(5):658-661WU Qiang, ZHANG Baoyong, WANG Yongjing. Study of Decomposition Thermody Namics of Gas Hydrate[J].Journal of China University of Mining&Technology,2006, 35(5):658-661
[11]吴琼,吴强,张保勇,等.丙烷对瓦斯混合气水合物相平衡的影响[J].煤炭学报,2014, 39(7):1283-1288WU Qiong, WU Qiang, ZHANG Baoyong, et al. Effect of Propane on the Phase Equilibrium of Mixture Gas Hydrate[J]. Journal of China Coal Society, 2014, 39(7):1283-1288
[12] SURYA D, ALEXANDER G, ALLAN S M. THF-water Hydrate Crystallization:an Experimental Investigation[J]. Journal of Crystal Growth, 1999, 204(4):525-538
[13] SHARMA D, SOWJANYA Y, DHANUNJANA C V, et al. Methane Storage in Mixed Hydrates with Tetrahydrofuran[J].Indian of Chemical Technology, 2014, 21(21):114-119
[14] SHENG D, JOO Y L, CARLOS S. Hydrate Nucleation in Quiescent and Dynamic Conditions[J]. Fluid Phase Equilibria, 2014, 378:107-112
[15]叶楠.季盐类水合物相平衡条件及生长动力学研究[D].上海:上海交通大学,2014YE Nan. Equilibrium Conditions and Kinetics of Hydrates Forming with Quaternary Salts[D]. Shanghai:Shanghai Jiao Tong University, 2014
[16]许浪.瓦斯爆炸冲击波衰减规律及安全距离研究[D].徐州:中国矿业大学,2015XU Lang. Study on Phase Equilibrium Theoretical Predictions and Dynamic Characteristics of gas Hydrate in the Complex System Containing Thermodynamic Additives[D]. Xuzhou:China University of Mining and Technology, 2015
[17]孙国庆.THF和TBAB对煤层气水合物相平衡影响的实验及理论研究[D].太原:太原理工大学,2015SUN Guoqing. Experimental and Theoretical Research of the Effect of TBAB and THF on Coal-bed Methane Hydrate Phase Equilibrium[D]. Taiyuan:Taiyuan University of Technology, 2015
[18]周诗岽,余益松,王树立,等.管道流动体系下天然气水合物生成模型的研究进展[J].天然气工业,2014, 34(2):92-98ZHOU Shidong, YU Yisong, WANG Shuli, et al.Rescearch Progress in the Natural Gas Hydrate Formation Model Under the Pipe Flow System[J]. Natural Gas Industry, 2014, 34(2):92-98
[19]赵欣,邱正松,江琳,等.动力学抑制剂作用下天然气水合物生成过程的实验分析[J].天然气工业,2014, 34(2):105-110ZHAO Xin, QIU Zhengsong, JIANG Lin, et al. An Experimental Analysis of Natural Gas Hydrate Formationat the Presence of Kinetic Hydrate Inhibitors[J]. Natural Gas Industry, 2014, 34(2):105-110
[20]梁德青,臧小亚,吴能友.介观孔隙中天然气水合物生成过程模拟[J].天然气工业,2013, 33(7):24-28LIANG Deqing, ZANG Xiaoya, WU Nengyou. A Simulation Study of Natural Gas Hydrate Generation in Mesoscopic-scale Pores[J]. Natural Gas Industry, 2013,33(7):24-28
[21]金学彬,陈强,邢兰昌,等.多孔介质中甲烷水合物聚散过程的交流阻抗谱响应特征[J].天然气工业,2016, 36(3):120-127JIN Xuebin, CHEN Qiang, XING Lanchang, et al. Response Characteristics of AC Impedance Spectroscopy During the Formation and Dissociation of Methane Hydrate in Porous Media[J]. Natural Gas Industry, 2016,36(3):120-127
[22]任静雅,鲁晓兵,张旭辉.水合物沉积物电阻特性研究初探[J].岩土工程学报,2013, 35(1):161-165REN Jingya, LU Xiaobing, ZHANG Xuhui. Preliminary Study on Electric Resistance of Hydrate-bearing Sediments[J]. Chinese Journal of Geotechnical Engineering,2013, 35(1):161-165
[23] ZATSEPINA O Y, BUFFETT B A. Nucleation of CO_2-hydrate in a Porous Medium[J]. Fluid Phase Equilibria,2002, 200(2):263-275
[24] SLOAN E D, FFLEYFEL J R. A Molecular Mechanism for Gas Hydrate Nucleation From Ice[J]. AIChE Journal,1991, 37(9):146-151
[25] CHRISTIANSEN R L, SLOAN E D. Mechanisms and Kinetics of Hydrate Formation[J]. Annals of the New York Academy of Sciences, 1994, 715(1):283-305
[26]陈光进,孙长宇,马庆兰.气体水合物科学与技术[M].北京:化学工业出版社,2007CHEN Guangjin, SUN Changyu, MA Qinglan. Scientific and Technology of Gas Hydrate[M]. Beijing:Chemical Industry Publishing House, 2007
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