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Pyrolysis is an important technology in the utilization of low‐rank coals (LRCs) and is a prerequisite stage for other conversion methods. This study aimed to develop an understanding of the pyrolysis process of LRCs, especially the relationship between the pyrolysis kinetics and the internal chemical structure. The chemical structure parameters of all of the samples were obtained using the Fourier transform infrared spectroscopy (FTIR) method. Thermogravimetric (TG) experiments were conducted at different heating rates (5, 10, and 20 K/min), and the experimental results were fitted using the distributed activation energy model (DAEM). DAEM based on double‐Gaussian distribution (2G‐DAEM) exhibited an acceptable fit to the experimental data in this study. An analysis of the chemical structure parameters of the four types of coals and the kinetic model obtained by fitting indicated that the difference in the chemical structure parameters among the coal samples could effectively explain the difference in the pyrolysis process and the activation energy distribution. The primary pyrolysis stage of the coal samples, including the thermal hysteresis effect caused by the increase in the heating rate, was accurately described by the 2G‐DAEM in this study. 相似文献
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利用热重-红外分析仪(TG-FTIR)研究了手机SIM卡在不同升温速率下的热解行为,探讨了升温速率对热解参数及热解产物的影响。采用分布式活化能模型求解了热解活化能,探讨了活化能随转化率的变化规律。研究结果表明:手机SIM卡呈现一段热解,主要热解温区在350~500 ℃,最大失重速率为?62.57%/min,总失重率高达90%。随着升温速率的提高,热解初始温度和热解结束温度均增大,最大热解速率和对应的温度也都增大;热解活化能在170~204 kJ/mol变化,随转化率变化规律呈现先增大后减小再增大后逐渐减小的规律,在转化率0.2时达到最大值;主要热解产物为苯、烷烯烃等可燃成分,而且含有氯、氮等元素;升温速率对热解组分没有影响。 相似文献
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研究了不同压力、升温速率以及添加CaO催化剂对松木屑热解过程的影响并进行了动力学分析。研究结果表明:1)增加系统的反应压力会降低热解过程的最终失重率,最终的剩余物质增加,并且提高反应压力,不利于挥发分析出。但是通过动力学分析发现,一定范围内增加压力能够降低热解过程中的活化能,从而有利于热解反应的发生,但是压力超过0.7 MPa以后,活化能开始增加。2)增加升温速率,挥发分释放的越强烈,有利于热解反应的进行,但挥发分大量析出的温度范围并没有很明显的浮动。通过动力学分析发现,随着升温速率增加,反应的活化能出现减少趋势,这说明随着升温速率增加,松木屑热解反应更加激烈。3)在松木屑热解反应中添加CaO对反应过程有较大的影响。随着CaO催化剂添加量增加,松木屑最终失重率逐渐减少,从72.81 %减少到59.61 %,降幅达到18.13 %。DTG曲线显示失重峰增加到4个,另外两个为Ca(OH)2和CaCO3分解所引起的失重峰。随着CaO添加量的增加,第1个失重峰的峰值和第2个失重峰的峰值逐渐减小,最大峰值对应的温度点变化不明显;第3、第4个失重峰的峰值逐渐增加,最大峰值对应的温度出现明显增加趋势。 相似文献
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果壳生物质热解特性与动力学 总被引:1,自引:0,他引:1
采用热重分析仪对林产果壳生物质(澳洲坚果壳、油茶壳、核桃壳)热解特性进行了研究,利用分布活化能模型(DAEM)分析了热解动力学。热解特性研究表明:油茶壳最大失重速率最小,热解起始温度、结束温度、最大失重速率温度均低于澳洲坚果壳和核桃壳;澳洲坚果壳和核桃壳热解特征值近似;3种果壳生物质随升温速率的增加,热解过程向高温区转移。DAEM研究表明:DAEM适用于3种果壳生物质的热解动力学研究,相关系数R2在0.914~0.999之间;澳洲坚果壳热解活化能83.91~211.86 kJ/mol,油茶壳热解活化能68.64~244.49 kJ/mol,核桃壳热解活化能98.69~267.75 kJ/mol;随转化率的增加,3种果壳生物质活化能呈现相同的变化趋势,但变化幅度不同。 相似文献
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Pyrolysis of sawdust and its three components (cellulose, hemicellulose and lignin) were performed in a thermogravimetric analyzer (TGA92) under syngas and hydrogen. The effect of different heating rates (5, 10, 15 and 20 °C/min) on the pyrolysis of these samples were examined. The pyrolysis tests of the synthesized samples (a mixture of the three components with different ratios) were also done under syngas. The distributed activation energy model (DAEM) was used to study the pyrolysis kinetics. It is found that syngas could replace hydrogen in hydropyrolysis process of biomass. Among the three components, hemicellulose would be the easiest one to be pyrolyzed and then would be cellulose, while lignin would be the most difficult one. Heating rate could not only affect the temperature at which the highest weight loss rate reached, but also affect the maximum value of weight loss rate. Both lignin and hemicellulose used in the experiments could affect the pyrolysis characteristic of cellulose while they could not affect each other obviously in the pyrolysis process. Values of k0 (frequency factor) change very greatly with different E (activation energy) values. The E values of sawdust range from 161.9 to 202.3 kJ/mol, which is within the range of activation energy values for cellulose, hemicellulose and lignin. 相似文献
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The pyrolysis behavior of two kinds of typical biomass (pine wood and cotton stalk) was studied in nitrogen atmosphere at various heating rates by thermogravimetric analysis (TGA). The pyrolysis process can be divided into three stages: evolution of moisture (<200℃), devolatilization (200~400℃) and carbonization (>400℃). The comparison of DTG curves of two biomass materials show that the higher the hemicellulose content of biomass, the more evident the shoulder peak of DTG curve. The weight loss process of two materials was simulated by the kinetic model assuming cellulose, hemicellulose and lignin pyrolyzing independently and in parallel, obeying first-order reactions. The pyrolysis kinetic parameters corresponding to the three components were estimated by the nonlinear least square algorithm. The results show that their fitting curves are in good agreement with the experimental data. Their activation energy values for pine wood and cotton stalk are in the range of 188~215, 90~102, 29~49 and 187~214, 95~101, 30~38 kJ/mol, respectively. The corresponding pre-exponential factors are in the range of 1.8′1015~2.0′1016, 1.6′107~7.1′108, 9.3′101~1.5′103 and 1.2′1015~6.7′1017, 1.2′108~1.4′109, 1.4′102~4.6′102 min-1, respectively. In addition, the activation energy of cellulose and lignin increased and their contributions to volatile tended to fall, whereas the activation energy of hemicellulose decreased and its contribution to volatile tended to rise with increasing of heating rate. 相似文献
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利用热重红外联动技术(TG-DTG-FTIR)研究了橡胶籽油中的单不饱和游离脂肪酸油酸组分在不同升温速率(5℃/min、10℃/min、20℃/min、30℃/min)下的热解特性。然后,用多元线性回归法对油酸非等温热解所得到的特性参数进行研究并计算,求得不同升温速率下对应的反应级数、活化能和指前因子,并对不同升温速率下油酸热解反应活化能和指数前因子作线性拟合。结果表明:油酸热解过程主要可分为0~268℃和268~300℃两个阶段,由红外谱图特征峰的分析可知,不同升温速率下,在油酸热解的阶段内均出现了水蒸气、CH4、CO2和CO这4种主要气体挥发分。随着升温速率的增大,油酸热解的最大失重速率随之增大,热解区间也向着高温段移动,同时计算在升温速率从5~30℃/min的过程中,反应级数n=1时,热解反应活化能由105.57kJ/mol降低至93.99kJ/mol,指数前因子由6.99×106降低至6.7×105;n≠1时,热解反应活化能由102.45kJ/mol降低至93.38kJ/mol,指数前因子由3.13×106降低至2.97×104,反应活化能和指数前因子随升温速率的增大出现明显减小。通过对不同升温速率下油酸热解反应的活化能和指数前因子进行线性拟合后发现,两者间具有较好的补偿效应。 相似文献
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Je‐Lueng Shie Ching‐Yuan Chang Jyh‐Ping Lin Chao‐Hsiung Wu Duu‐Jong Lee 《Journal of chemical technology and biotechnology (Oxford, Oxfordshire : 1986)》2000,75(6):443-450
Oil sludge, if unused, is one of the major industrial wastes requiring treatment from petroleum refinery plants or the petrochemical industry. It contains a large amount of combustibles with high heating values. The treatment of waste oil sludge by burning has certain benefits; however, it cannot provide the useful resource efficiently. On the other hand, the conversion of oil sludge to lower molecular weight organic compounds by pyrolysis not only solves the disposal problem but also has the appeal of resource utilization. The major sources of oil sludge include the oil storage tank sludge, the biological sludge, the dissolve air flotation (DAF) scum, the American Petroleum Institute (API) separator sludge and the chemical sludge. In this study, the oil sludge from the oil storage tank of a typical petroleum refinery plant located in northern Taiwan is used as the raw material of pyrolysis. Its heating value of dry basis and low heating value of wet basis are about 10681 kcal kg−1 and 5870 kcal kg−1, respectively. The removal of the moisture from oil sludge significantly increases its heating value. The pyrolysis of oil sludge is conducted by the use of nitrogen as the carrier gas in the temperature range of 380–1073 K and at various constant heating rates of 5.2, 12.8 and 21.8 K min−1. The pyrolytic reaction is significant at 450–800 K and complex. For the sake of simplicity and engineering use, a one‐reaction kinetic model is proposed for the pyrolysis of oil sludge, and is found to satisfactorily fit the experimental data. The activation energy, reaction order and frequency factor of the corresponding pyrolysis reaction in nitrogen for oil sludge are 78.22 kJ mol−1, 2.92 and 9.48 × 105 min−1, respectively. For precise use, the two‐ and three‐reaction models are proposed to describe the pyrolysis results. Among the three models proposed, the three‐reaction model gives the best fit. These results are very useful for the proper design of the pyrolysis system of the oil sludge under investigation. © 2000 Society of Chemical Industry 相似文献
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The product distribution and kinetic analysis of low-rank coal vitrinite were investigated during the chemical looping gasification (CLG) process.The acid washing method was used to treat low-rank coal,and the density gradient centrifugation method was adopted to obtain the coal macerals.By combining thermogravimetric analysis and online mass spectrometry,the influence of the heating rate and oxygen carrier (Fe2O3) blending ratio on product distribution was discussed.The macroscopic kinetic parameters were solved by the Kissinger-Akahira-Sunose (KAS) method,and the main gaseous product formation kinetic parameters were solved by the iso-conversion method.The results of vitrinite during slow heating chemical looping gasification showed that the main weight loss interval was 400-600 ℃,and the solid yield of sample vitrinite-Fe-10 at different heating rates was 64.30%-69.67%.When β =20 ℃·min-1,the maximum decomposition rate of vitrinite-Fe-10 was-0.312%·min-1.The addition of Fe2O3 reduced the maximum decomposition rate,but by comparing the chemical looping conversion characteristic index,it could be inferred that the chemical looping gasification of vitrinite might produce volatile sub-stances higher than the pyrolysis process of vitrinite alone.The average activation energy of the reaction was significantly reduced during chemical looping gasification of vitrinite,which was lower than the average activation energy of 448.69 kJ·mol-1 during the pyrolysis process of vitrinite alone.The gaseous products were mainly CO and CO2.When the heating rate was 10 ℃·min-1,the highest activation energy for CH4 formation was 21.353 kJ·mol-1,and the lowest activation energy for CO formation was 9.7333 kJ·mol-1.This study provides basic data for exploring coal chemical looping gasification mecha-nism and reactor design by studying the chemical looping gasification process of coal macerals. 相似文献
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PVC木塑复合材料热解动力学 总被引:2,自引:0,他引:2
将木粉按一定比例添加到PVC中得到复合材料,通过热重分析研究复合材料在空气、N2气氛下不同升温速率时的热解行为。通过Doyle和Tang method法计算了木塑材料的降解活化能。利用活化能分布函数,分析了复合材料在热解、燃烧过程中不同阶段的反应活性变化规律。研究表明,热解过程可分为3个阶段,230~360℃为第一失重阶段,360~430℃为稳定阶段,430~580℃为第二失重阶段。升温速率及反应气氛对热解过程有显著影响。由分布活化能模型计算表明,其热解动力学为一级反应,两个失重阶段的活化能分别为220kJ·mol-1和139kJ·mol-1,反应活性随失重率的增加而减少。 相似文献
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《Fuel Processing Technology》2001,69(1):1-12
Hydrothermal water treatments and supercritical (SC) water treatments of a lignite were performed to examine the feasibility of upgrading low-rank coals. The treatment below 400°C was found to be effective enough to keep high gasification reactivity at high temperature, as well as to suppress spontaneous combustion. The pyrolysis and gasification behaviors of raw and pretreated coals were examined by thermogravimetry (TG). The kinetic analysis was carried out based on a new distributed activation energy model (DAEM) presented by Miura [K. Miura, Energy & Fuels, (12), 864–869 (1998).]. According to this method, thermogravimetric curves measured at two or more different heating rates were needed to obtain the activation energy distribution function f(E) of a given coal sample. It was found that in the case of pyrolysis, the peak values of f(E) curves for upgraded coal samples are nearly 300 kJ/mol, whereas, the peak value of f(E) curve for their parent coal is about 200 kJ/mol. In the case of gasification, where only single reactions occur, the application of this new DAEM can give the changes of activation energy during reaction. Some interesting results occur, which may hint at some changes in the rate-controlling step of reaction or in the physical structure of coal during gasification. 相似文献
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《Fuel》2006,85(5-6):664-670
The devolatilization characteristics of biomass (wheat straw, coconut shell, rice husk and cotton stalk) during flash pyrolysis has been investigated on a plasma heated laminar entrained flow reactor (PHLEFR) with average heating rates of 104 K/s. These experiments were conducted with steady temperatures between 750 and 900 K, and the particle residence time varied from about 0.115 to 0.240 s. The ash tracer method was introduced to calculate the yield of volatile products at a set temperature and the residence time. This experimental study showed that the yield of volatile products depends both on the final pyrolysis temperature and the residence time. From the results, a comparative analysis was done for the biomasses, and a one-step global model was used to simulate the flash pyrolytic process and predict the yield of volatile products during pyrolysis. The corresponding kinetic parameters of the biomasses were also analyzed and determined. These results were essential for designing a suitable pyrolysis reactor. 相似文献