Behaviors of hydrogen bonds formed by lignite and aromatic solvents in direct coal liquefaction: Combination analysis of density functional theory and experimental methods
Behaviors of hydrogen bonds formed by lignite and aromatic solvents in direct coal liquefaction: Combination analysis of density functional theory and experimental methods
复制标题
煤直接液化过程中褐煤与芳烃溶剂形成氢键的行为：密度泛函理论与实验方法的结合分析
DOI：
10.1016/j.fuel.2020.117011
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发表时间：
2020-04
期刊：
影响因子：
7.4
通讯作者：
Wen Li
中科院分区：
文献类型：
--
作者：
Ranran Hou;Zongqing Bai;Hongyan Zheng;Zhihao Feng;Donghong Ye;Zhenxing Guo;Lingxue Kong;Jin Bai;Wen Li
氢键丰度高，对轻质产物的生成影响大，在低变质煤的热转化过程中起着至关重要的作用，尤其是煤直接液化(DCL)。用原位漫反射红外傅里叶变换(DRIFT)分析了氢键的相对分布，用密度泛函理论(DFT)和约化密度梯度法(RDG)可视化分析了煤与溶剂之间的氢键(特别是OH-π)。在200℃、250℃和300℃下，对脱矿云南褐煤(Deyn)加/不加苯进行了DCL实验，并用固体~(13)C核磁共振和原位漂移研究了含氧官能团。随着温度的升高，OH-π氢键的相对含量增加。与四氢萘(THN)相比，苯是更强的氢键受体。DCL实验得出的结论与密度泛函理论计算相一致。具体地说，质量浓度为2%的苯促进了O-H键、羧基的裂解和芳基醚键的生成，并且随着DCL温度的升高，苯引起的差异加剧。
Hydrogen bonds play a crucial role in thermal conversion of low rank coal, especially direct coal liquefaction (DCL) because of their wealthy abundance and great influence on generation of light products. Relative distribution of hydrogen bonds was evaluated with in-situ diffuse reflectance infrared Fourier transformation (DRIFT), while visualization analysis of hydrogen bonds (OH-π in particular) between coal and solvents were performed using density functional theory (DFT) and reduced density gradient (RDG) analysis. In terms of their effects, DCL experiments of demineralized Yunnan lignite (DeYN) with/without addition of benzene at 200, 250 and 300 °C were carried out, and oxygen-containing functional groups were investigated by solid-state13C NMR and in-situ DRIFT. Relative content of OH-π hydrogen bonds increased with temperature rising. Benzene is the stronger hydrogen bonds acceptor compared to tetralin (THN). Conclusions drawn from DCL experiments are consistent with DFT calculations. To be specific, benzene with mass concentration of 2% promotes cleavage of O–H bonds, carboxyl groups and the generation of aryl ether bonds, and the differences caused by benzene are intensified when DCL temperature rises.
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影响因子：
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作者：
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