Characterization of organonitrogen species in Xianfeng lignite by sequential extraction and ruthenium ion-catalyzed oxidation
Characterization of organonitrogen species in Xianfeng lignite by sequential extraction and ruthenium ion-catalyzed oxidation
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顺序萃取和钌离子催化氧化表征先锋褐煤中的有机氮形态
DOI：
10.1016/j.fuproc.2014.05.004
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发表时间：
2014-10-01
影响因子：
7.5
通讯作者：
Zhao, Yun-Peng
中科院分区：
文献类型：
--
作者：
Liu, Fang-Jing;Wei, Xian-Yong;Zhao, Yun-Peng
对先锋褐煤(XL)进行了连续超声提取(UE)、连续热提取(TE)和RICO(RICO)三步降解，以表征XL中的有机氮物种(ONSS)。X-射线光电子能谱分析表明，XL和UE残渣中的氮形态主要是吡咯、氨基和季氮化合物，而TE残渣中的氮主要是硝基芳烃、化学吸附的N-氧化物和吡咯氮。GC/MS分析表明，UE渣油萃取物中含有吡啶类、喹啉类、苯并[d]咪唑类和芳香胺类化合物。在有机氮化合物中，吡啶类和喹啉类化合物含量最高。在UE残基的TE过程中，ONSS可以通过热破坏非共价键，如氢键和芳香族pi-pi相互作用来释放。含氮大分子芳烃在XL基质(XLm)中的降解生成了TE残渣中RICO释放的大部分ONSS。硝基苯羧酸是TE残基中RICO释放出的最丰富的ONSS，应通过大分子硝基芳香族化合物在XLM中的降解而释放。(C)2014爱思唯尔B.V.保留所有权利。
A three-step degradation, including sequential ultrasonic extraction (UE), sequential thermal extraction (TE), and ruthenium ion-catalyzed oxidation (RICO), of Xianfeng lignite (XL) was performed to characterize the organonitrogen species (ONSs) in XL More than 87.3% of organic matter in XL was converted into soluble portions through the degradation. The analysis with X-ray photoelectron spectrometer shows that pyrrolic, amino, and quaternary nitrogen species are the main nitrogen forms both in XL and its residue from UE, while nitroaromatics, chemisorbed N-oxides, and pyrrolic nitrogen are predominant in the residue from TE. A series of ONSs, including pyridines, quinolines, benzo[d]imidazoles, and arylamines, were identified in the extracts from TE of the UE residue according to GC/MS analysis. Among the ONSs, pyridines and quinolines are the most abundant. The ONSs could be released by thermally destroying noncovalent bonds, such as hydrogen bonds and aromatic pi-pi is interactions, during TE of the UE residue. Most of ONSs released from RICO of the TE residue could be generated from the degradation of nitrogen-containing macromolecular aromatics in XL matrix (XLM). Nitrobenzenecarboxylic acids are the most abundant ONSs released from RICO of the TE residue and should be released by the degradation of macromolecular nitroaromatics in XLM. (C) 2014 Elsevier B.V. All rights reserved.