Coal pyrolysis characteristics by TG–MS and its late gas generation potential
Coal pyrolysis characteristics by TG–MS and its late gas generation potential
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TG-MS 煤热解特性及其后期产气潜力
DOI：
10.1016/j.fuel.2015.04.055
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发表时间：
2015-09
期刊：
影响因子：
7.4
通讯作者：
Haitao Xue
中科院分区：
文献类型：
--
作者：
Min Wang;Zhongsheng Li;Wenbiao Huang;Jinxiu Yang;Haitao Xue
近年来，随着深层天然气开采的日益成功，对深层有机质生气潜力的评价，特别是晚期生气潜力的评价越来越受到重视。本文利用热重-质谱（TG-MS）联用技术研究了松辽盆地煤热解过程中烃类和非烃类的成气过程、成气特征及其后期成气潜力。TG-MS实验结果表明：（1）在升温速率为10 °C/min的条件下，煤热解过程中甲烷的生成开始于~ 300 °C，在480 °C时达到峰值，在~ 850 °C时结束，远高于其它烃类的终止生成温度;（2）通过离子碎片产气曲线考察甲烷生成特性时，当质荷比m/z =15时，比目前使用的m/z =16时得到更精确的结果;（3）该煤具有较高的晚期生气潜力，在600 °C以后的晚期阶段产生了17%的额外甲烷（相当于镜质体反射率：Ro = 2.5%），并且甲烷生成在5.3%（Ro）的成熟度水平处结束。利用煤热解结果进行标定后，建立了动力学模型，并成功地应用于徐家围子断陷沙河子组天然气的生成时间和生成机理的研究。动力学模型计算结果表明，沙河子组天然气的生成时间为1115 ~ 50 Ma，甲烷生成稳定，没有出现主要的生成高峰，持续时间为165 Ma。
As natural gas production from deep strata becomes increasingly successful in recent years, the evaluation on gas generation potential from OM (organic matter) in the deep formations is attracting increasing attention recently, especially the late gas generation potential. In this paper, a TG–MS (thermogravimetric analysis–mass spectrometry) device was applied to investigate the process and characteristics of gas generation of HCs (hydrocarbons) and non-HCs (non-hydrocarbons) during the pyrolysis processes of coal from Songliao Basin, and its late gas generation potential. The TG–MS experimental results show that: (1) during coal pyrolysis with heating rate of 10 °C/min, methane generation started at ∼300 °C, reached its peak generation at 480 °C, and ended at ∼850 °C, which was much higher than the ending generation temperatures of other HCs; (2) when investigating the methane generation characteristics through the gas generation curve by ion fragments, more accurate results are obtained with mass to charge ratiom/z =15 than currently usedm/z =16; (3) this coal has a high late gas generation potential, with 17% additional methane generated at late generation stage after 600 °C (equivalent to a vitrinite reflectance: Ro ⩾ 2.5%), and the methane generation ended at a maturity level of 5.3% (Ro). After calibration with coal pyrolysis results, a kinetic model has been established and applied successfully to estimate gas generation timing and illustrate gas generation mechanisms of the Shahezi Formation in the Xujiaweizi Fault Depression. Based on the results derived from the proposed kinetic model, the gas generation timing for the Shahezi Formation was between ∼115 and 50 Ma, and methane appeared to be generated steadily without any major generation peak indentified during this period and the gas generation lasted for ∼65 Ma.
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