

浏览全部资源
扫码关注微信
1. 宁夏大学省部共建煤炭高效利用与绿色化工国家重点实验室,化学化工学院,宁夏 银川 750021
2. 宁夏庆华煤化集团有限公司,宁夏 吴忠 751100
Received:10 October 2019,
Revised:2019-11-08,
Online First:14 August 2020,
Published:05 February 2020
移动端阅览
毛宁, 王强, 杨妍, 徐敦信, 冯炜, 张金鹏, 白红存, 郭庆杰. 基于显微组分化学键特征的宁夏庆华煤热解特性及动力学分析[J]. 化工学报, 2020, 71(2): 811-820
MAO Ning, WANG Qiang, YANG Yan, XU Dunxin, FENG Wei, ZHANG Jinpeng, BAI Hongcun, GUO Qingjie. Pyrolysis characteristics and kinetics analysis of Qinghua coal, Ningxia based on chemical bonding characteristics of macerals[J]. CIESC Journal, 2020, 71(2): 811-820
毛宁, 王强, 杨妍, 徐敦信, 冯炜, 张金鹏, 白红存, 郭庆杰. 基于显微组分化学键特征的宁夏庆华煤热解特性及动力学分析[J]. 化工学报, 2020, 71(2): 811-820 DOI: 10.11949/0438-1157.20191156.
MAO Ning, WANG Qiang, YANG Yan, XU Dunxin, FENG Wei, ZHANG Jinpeng, BAI Hongcun, GUO Qingjie. Pyrolysis characteristics and kinetics analysis of Qinghua coal, Ningxia based on chemical bonding characteristics of macerals[J]. CIESC Journal, 2020, 71(2): 811-820 DOI: 10.11949/0438-1157.20191156.
通过X射线光电子能谱和傅里叶红外光谱表征宁夏宁东庆华煤不同显微组分的官能团种类、表面结构元素价态分布及化学键赋存特征。采用热重-质谱联用考察庆华煤镜质组和惰质组在不同热解温度下的失重行为和关键气体组分变化。进一步基于Coats-Redfern模型从化学键断裂特征和反应动力学角度探讨煤镜质组和惰质组的热解行为差异。结果表明,庆华煤显微组分的热解失重峰与相应化学键断裂信息能够很好地吻合。不同显微组分的热重曲线变化趋同,但相同热解温度下镜质组的失重率始终高于惰质组。快速热解阶段镜质组较惰质组表现出更大的失重率和最大失重速率。其主要原因在于镜质组的脂肪族官能团相对含量更高,快速热解阶段会发生更多的C
al
—C
al
断裂。不同热解温度下庆华煤显微组分三个主要热解阶段的活化能和频率因子大小次序为:
快速热解阶段
>
快速缩合阶段
>
缓慢热解阶段。在快速热解阶段,镜质组和惰质组的平均活化能均约为75 kJ/mol,但镜质组的频率因子更高。
X-Ray photoelectron spectroscopy and Fourier transform infrared spectroscopy were used to characterize the functional group types
surface structure element valence distribution and chemical bond occurrence characteristics of Ningxia Ningdong Qinghua coal. Then the mass loss behavior of vitrinite and inertinite of Qinghua coal at different pyrolysis temperatures and the changes of key gas components were investigated by means of the thermogravimetry coupled with mass spectrometry (TG-MS). Furthermore
the differences of pyrolysis behavior between vitrinite and inertinite were discussed from the point of view of chemical bonding breaking and pyrolysis kinetics based on Coats-Redfern model. The results show that the pyrolysis weightlessness peaks of Qinghua coal macerals at different temperatures are in good agreement with the information of corresponding chemical bond breaking. The TG curves of different macerals of Qinghua coal are similar
but the mass loss rate of vitrinite is always higher than that of inertinite at the same pyrolysis temperature. In the fast pyrolysis stage
vitrinite exhibits greater mass loss rate and also maximum mass loss rate than inertinite. The main reason is that the relative content of aliphatic functional groups in vitrinite is higher
and more C
al
—C
al
bonds would break down during the fast pyrolysis stage. The order of activation energy and frequency factor of three main pyrolysis stages of Qinghua coal macerals at different pyrolysis temperatures is: fast pyrolysis stage
>
fast polycondensation stage
>
slow pyrolysis stage. In the fast pyrolysis stage
the average activation energies of vitrinite and inertinite are both about 75 kJ/mol
but the frequency factor of vitrinite is higher.
Li P , Zong Z M , Wei X Y , et al . Structural features of liquefaction residue from Shenmu-Fugu subbituminous coal [J ] . Fuel , 2019 , 242 : 819 - 827 .
史航 , 靳立军 , 魏宝勇 , 等 . 大柳塔煤及显微组分在不同气氛下的热解行为 [J ] . 煤炭学报 , 2019 , 44 ( 1 ): 316 - 322 .
Shi H , Jin L J , Wei B Y , et al . Pyrolysis behavior of Daliuta coal and its macerals under different atmospheres [J ] . Journal of China Coal Society , 2019 , 44 ( 1 ): 316 - 322 .
赵云鹏 , 胡浩权 , 靳立军 , 等 . 矿物质对不同还原程度煤显微组分半焦燃烧特性影响 [J ] . 化工学报 , 2019 , 70 ( 8 ): 2946 - 2953 .
Zhao Y P , Hu H Q , Jin L J , et al . Effect of minerals on semi-coke combustion characteristics of maceral with different reducibility [J ] . CIESC Journal , 2019 , 70 ( 8 ): 2946 - 2953 .
Roberts M J , Everson R C , Neomagus H W J P , et al . The characterisation of slow-heated inertinite- and vitrinite-rich coals from the South African coalfields [J ] . Fuel , 2015 , 158 ( 5 ): 591 - 601 .
Yang Q , Chang H , Du S , et al . Pyrolysis interaction between vitrinite and inertinite from Chinese Wucaiwan coal [J ] . Journal of Fuel Chemistry and Technology , 2015 , 24 ( 4 ): 405 - 418 .
Chang H , Deng H , Yang Q , et al . Interaction of vitrinite and inertinite of Bulianta coal in pyrolysis [J ] . Fuel , 2017 , 207 ( 3 ): 643 - 649 .
Wang S , Tang Y , Schobert H H , et al . FTIR and simultaneous TG/MS/FTIR study of Late Permian coals from Southern China [J ] . Journal of Analytical and Applied Pyrolysis , 2013 , 100 ( 2 ): 75 - 80 .
Das T K . Evolution characteristics of gases during pyrolysis of maceral concentrates of Russian coking coals [J ] . Fuel , 2001 , 80 ( 4 ): 489 - 500 .
Das T K . Thermogravimetric characterisation of maceral concentrates of Russian coking coals [J ] . Fuel , 2001 , 80 ( 1 ): 97 - 106 .
Wang J , Du J , Chang L , et al . Study on the structure and pyrolysis characteristics of Chinese western coals [J ] . Fuel Processing Technology , 2010 , 91 ( 4 ): 430 - 433 .
Sun Q , Li W , Li B Q . The synergistic effect between macerals during pyrolysis [J ] . Fuel , 2002 , 81 ( 7 ): 973 - 974 .
Sun Q , Li W , Chen H , et al . Thermogravimetric-mass spectrometric study of the pyrolysis behavior of Shenmu macerals under hydrogen and argon [J ] . Energy Sources , Part A , 2006 , 28 ( 14 ): 1281 - 1294 .
Sun Q , Li W , Chen H , et al . Devolatilization characteristics of Shenmu coal macerals and kinetic analysis [J ] . Energy Sources , Part A , 2006 , 28 ( 9 ): 865 - 874 .
Sun Q , Li W , Chen H . The synergistic effect between coal macerals during hydropyrolysis [J ] . Energy Sources , 2007 , 29 ( 2 ): 125 - 132 .
Zhao Y , Hu H , Jin L , et al . Pyrolysis behavior of vitrinite and inertinite from Chinese Pingshuo coal by TG–MS and in a fixed bed reactor [J ] . Fuel Processing Technology , 2011 , 92 ( 4 ): 780 - 786 .
杨群 , 常海洲 , 杜帅 , 等 . 五彩湾煤镜质组与惰质组在热解中的相互作用 [J ] . 燃料化学学报 , 2015 , 43 ( 11 ): 1295 - 1302 .
Yang Q , Chang H Z , Du S , et al . Pyrolysis interaction between vitrinite and inertinite from Chinese Wucaiwan coal [J ] . Journal of Fuel Chemistry and Technology , 2015 , 43 ( 11 ): 1295 - 1302 .
Feng Z , Bai Z , Zheng H , et al . Study on the pyrolysis characteristic of mild liquefaction solid product of Hami coal and CO 2 gasification of its char [J ] . Fuel , 2019 , 253 : 1034 - 1041 .
冯炜 , 高红凤 , 王贵 , 等 . 枣泉煤分子模型构建及热解的分子模拟 [J ] . 化工学报 , 2019 , 70 ( 4 ): 1522 - 1531 .
Feng W , Gao H F , Wang G , et al . Molecular model and pyrolysis simulation of Zaoquan coal [J ] . CIESC Journal , 2019 , 70 ( 4 ): 1522 - 1531 .
Yan J , Jiao H , Li Z , et al . Kinetic analysis and modeling of coal pyrolysis with model-free methods [J ] . Fuel , 2019 , 241 : 382 - 391 .
Casal M D , Vega M F , Diaz-Faes E , et al . The influence of chemical structure on the kinetics of coal pyrolysis [J ] . International Journal of Coal Geology , 2018 , 195 : 415 - 422 .
Song H , Liu G , Zhang J , et al . Pyrolysis characteristics and kinetics of low rank coals by TG-FTIR method [J ] . Fuel Processing Technology , 2016 , 157 : 454 - 460 .
邹达 , 白翔 , 李显 , 等 . 新疆和丰煤分段热解过程中产物组成的演变规律 [J ] . 煤炭学报 , 2018 , 43 ( 3 ): 846 - 854 .
Zou D , Bai X , Li X , et al . Composition and structure evolution characteristics of product from segmenting pyrolysis of Xinjiang Hefeng coal [J ] . Journal of China Coal Society , 2018 , 43 ( 3 ): 846 - 854 .
Lei S , Liu Q , Guo X , et al . Pyrolysis behavior and bonding information of coal — a TGA study [J ] . Fuel Processing Technology , 2013 , 108 ( 6 ): 125 - 132 .
Zhang L , Hower J C , Liu W L . Non-isothermal TG-DSC study on prediction of caking properties of vitrinite-rich concentrates of bituminous coals [J ] . Fuel Processing Technology , 2017 , 156 : 500 - 504 .
Wang Y G , Wei X Y , Wang S K , et al . Structural evaluation of Xiaolongtan lignite by direct characterization and pyrolytic analysis [J ] . Fuel Processing Technology , 2016 , 144 : 248 - 254 .
Zhou Y , Li L , Jin L , et al . Pyrolytic behavior of coal-related model compounds connected with C—C bridged linkages by in - situ pyrolysis vacuum ultraviolet photoionization mass spectrometry [J ] . Fuel , 2019 , 241 : 533 - 541 .
李首毅 , 林雄超 , 鲁倍倍 , 等 . 矿物质对高碱煤显微组分热解特性的影响 [J ] . 化工进展 , 2019 , 38 ( 8 ): 3650 - 3657 .
Li S Y , Lin X C , Lu B B , et al . Effects of minerals on pyrolysis characteristics of maceral in high-alkali coal [J ] . Chemical Industry and Engineering Progress , 2019 , 38 ( 8 ): 3650 - 3657 .
Shi Z , Jin L , Zhou Y , et al . Online analysis of initial volatile products of Shenhua coal and its macerals with pyrolysis vacuum ultraviolet photoionization mass spectrometry [J ] . Fuel Processing Technology , 2017 , 163 : 67 - 74 .
Jin L , Han K , Wang J , et al . Direct liquefaction behaviors of Bulianta coal and its macerals [J ] . Fuel Processing Technology , 2014 , 128 : 232 - 237 .
Han F , Meng A , Li Q , et al . Thermal decomposition and evolved gas analysis (TG-MS) of lignite coals from Southwest China [J ] . Journal of the Energy Institute , 2016 , 89 ( 1 ): 94 - 100 .
Zou C , Ma C , Zhao J , et al . Characterization and non-isothermal kinetics of Shenmu bituminous coal devolatilization by TG-MS [J ] . Journal of Analytical and Applied Pyrolysis , 2017 , 127 : 309 - 320 .
Xu Y , Zhang Y , Wang Y , et al . Gas evolution characteristics of lignite during low temperature pyrolysis [J ] . Journal of Analytical and Applied Pyrolysis , 2013 , 104 : 625 - 631 .
常海洲 , 王传格 , 曾凡桂 , 等 . 不同还原程度煤显微组分组表面结构XPS对比分析 [J ] . 燃料化学学报 , 2006 , 34 ( 4 ): 389 - 394 .
Chang H Z , Wang C G , Zeng F G , et al . XPS comparative analysis of coal macerals with different reducibility [J ] . Journal of Fuel Chemistry and Technology , 2006 , 34 ( 4 ): 389 - 394 .
Jayaraman K , Kok M V , Gokalp I . Thermogravimetric and mass spectrometric (TG-MS) analysis and kinetics of coal-biomass blends [J ] . Renewable Energy , 2017 , 101 : 293 - 300 .
Guo Z , Zhang L , Wang P , et al . Study on kinetics of coal pyrolysis at different heating rates to produce hydrogen [J ] . Fuel Processing Technology , 2013 , 107 : 23 - 26 .
Zhu C , Xie Q , Zhong J , et al . Effects of hydrothermal treatment on oxygen functional groups and pyrolysis characteristics of a vitrinite-rich low rank coal [J ] . Asia-Pacific Journal of Chemical Engineering , 2019 , 12 : 1 - 13 .
Niu Z , Liu G , Yin H , et al . Devolatilization behaviour and pyrolysis kinetics of coking coal based on the evolution of functional groups [J ] . Journal of Analytical and Applied Pyrolysis , 2018 , 134 : 351 - 361 .
Zhang L , Hower J C , Liu W . Devolatilization and kinetics of maceral concentrates of bituminous coals [J ] . Fuel Processing Technology , 2016 , 154 : 147 - 155 .
0
Views
0
下载量
7
CSCD
Publicity Resources
Related Articles
Related Author
Related Institution
京公网安备11010102001995号