Interactions between organic nitrogen and inorganic matter in the pyrolysis zone of underground coal gasification: Insights from controlled pyrolysis experiments
Interactions between organic nitrogen and inorganic matter in the pyrolysis zone of underground coal gasification: Insights from controlled pyrolysis experiments
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煤炭地下气化热解区有机氮与无机物的相互作用：受控热解实验的见解
DOI：
10.1016/j.energy.2017.06.130
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发表时间：
2017-09
期刊：
影响因子：
9
通讯作者：
Changmin Zhang
中科院分区：
文献类型：
--
作者：
Kangle Ding;Changmin Zhang
近年来，在煤炭地下气化（UCG）的现场试验中发现了多种含氮杂环化合物和无机氮物种，引起了人们对环境影响的关注。以咔唑为模型化合物，研究了煤基质中各种含氮化合物的生成动力学。在高压釜中对煤中的咔唑进行了有、无矿物质或其主要活性组分存在下的热解实验。根据实验数据，探讨了无机物的影响、反应机理和化学动力学。结果表明，水对咔唑的热破坏的影响可以忽略不计。然而，水和氧化铝的结合可能在N-O原子交换中起作用，导致新的氨形成机制。黄铁矿在咔唑裂解过程中表现出比其他矿物更高的反应活性。计算得到咔唑与无机物共热解的表观活化能为202 ~ 305 kJ/mol。根据无机物对咔唑裂解的影响，将UCG热解区进一步划分为正效应区、过渡区和负效应区。
In recent years, a variety of N-heterocyclic compounds and inorganic nitrogen species were identified during the field-scale experiment on underground coal gasification (UCG), leading to concerns about the environmental impact. In an attempt to unravel the kinetics responsible for the generation of various nitrogen compounds (NCs), carbazole is selected in this paper as a model organic nitrogen compound in coal matrix. Hydrous pyrolysis experiments on carbazole were conducted using an autoclave in the presence and absence of minerals or their main active components in coal. Effects of inorganic matter, reaction mechanism and chemical kinetics were investigated on the basis of the experimental data. The results demonstrate negligible influence of water on thermal destruction of carbazole. However, the combination of water and aluminium oxide may play a role in the N – O atom exchange, resulting in a new ammonia formation mechanism. Pyrite exhibits extremely higher reactivity during carbazole cracking than other minerals. The calculated apparent activation energies for carbazole co-pyrolysis with inorganic matter range from 202 to 305 kJ/mol. According to the influence of inorganic matter on carbazole cracking, the pyrolysis zone of UCG could be further divided into positive effect subzone, transition subzone and negative effect subzone.
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