神府煤热解过程中焦炭结构与挥发分形成的关系——对流动相和固定相影响的进一步认识,Fuel Processing Technology

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神府煤热解过程中焦炭结构与挥发分形成的关系——对流动相和固定相影响的进一步认识
Fuel Processing Technology ( IF 7.2 ) Pub Date : 2018-09-01 , DOI: 10.1016/j.fuproc.2018.07.022
Kai Xu , Song Hu , Yi Wang , Liangping Zhang , Sheng Su , Long Jiang , Jun Xu , Zhufeng Ouyang , Jun Xiang

摘要挥发分的形成与热解过程中焦炭的化学结构密切相关。本研究对神府煤在 435 °C 不同停留时间下热解得到的半焦、焦油和气体产物进行了分子水平的综合分析，旨在揭示导致化学物质演化的反应途径。煤/焦的结构。结果表明，CO2和CO是主要的热解气产物，推断低阶神府煤中有机氧含量较高。在热解的初始阶段，桥键，特别是杂原子桥键，如O、N和S的裂解，会在半焦中产生相对稳定的自由基。流动相中轻组分的相变和沥青质的分解与轻焦油脂肪族化合物的形成密切相关。在热解的中后期，极性自由基的热裂解和溶剂提取的化质体材料的分解对焦油的形成起主要作用。此外，煤/炭骨架结构的外围芳香结构裂解，发生二次反应（如甲基化和脱氢反应），会导致焦油（轻焦油和重焦油）和H2的形成。

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Relation between char structures and formation of volatiles during the pyrolysis of Shenfu coal: Further understanding on the effects of mobile phase and fixed phase

Abstract The formation of resultant volatiles is closely related with chemical structure of char during the pyrolysis process. In this study, all-components, that are semi-char, tar and gas product obtained by Shenfu coal pyrolyzed under various residence time at 435 °C were comprehensively analyzed at molecular level, aiming to reveal the reaction pathways responsible for the evolution of chemical structure of coal/char. The results showed that CO2 and CO were the predominant pyrolysis gas product which inferred high content of organic oxygen species in low-rank Shenfu coal. At the initial stage of pyrolysis, cracking of bridged bonds, especially heteroatom bridged bonds, such as O, N and S, would produce relatively stable radicals in semi-char. Phase change of light components and decomposition of asphaltene in mobile phase can be strongly related with light tar aliphatic compounds formation. At the middle and later stage of pyrolysis, thermal cracking of polar radicals and decomposition of solvent extracted metaplast materials made predominant contribution to tar formation. In addition, the cracking of peripheral aromatic structures of coal/char skeleton structure, through which secondary reaction (such as methylation and dehydrogenation reaction) took place, would result in tar (light tar and heavy tar) and H2 formation.

更新日期：2018-09-01

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