唐跃刚, 徐靖杰, 郇璇, 王绍清, 陈鹏翔. 云南小发路无烟煤基石墨烯制备与谱学表征[J]. 煤炭学报, 2020, 45(2). DOI: 10.13225/j.cnki.jccs.2019.0216
引用本文: 唐跃刚, 徐靖杰, 郇璇, 王绍清, 陈鹏翔. 云南小发路无烟煤基石墨烯制备与谱学表征[J]. 煤炭学报, 2020, 45(2). DOI: 10.13225/j.cnki.jccs.2019.0216
TANG Yuegang, XU Jingjie, HUAN Xuan, WANG Shaoqing, CHEN Pengxiang. Preparation and spectroscopic characterization of coal-based graphene from anthracite in Xiaofalu,Yunnan,China[J]. Journal of China Coal Society, 2020, 45(2). DOI: 10.13225/j.cnki.jccs.2019.0216
Citation: TANG Yuegang, XU Jingjie, HUAN Xuan, WANG Shaoqing, CHEN Pengxiang. Preparation and spectroscopic characterization of coal-based graphene from anthracite in Xiaofalu,Yunnan,China[J]. Journal of China Coal Society, 2020, 45(2). DOI: 10.13225/j.cnki.jccs.2019.0216

云南小发路无烟煤基石墨烯制备与谱学表征

Preparation and spectroscopic characterization of coal-based graphene from anthracite in Xiaofalu,Yunnan,China

  • 摘要: 为研究云南小发路无烟煤制备煤基石墨烯及其谱学特征,采用改良的 Hummers 氧化还原法制备煤基石墨烯,并综合利用透射电镜(TEM),X 射线衍射(XRD)、拉曼光谱(Raman)和傅里叶变换红外光谱(FT-IR)等表征手段对原煤以及过程产物的化学结构进行表征,结果表明高温石墨化显著改善了小发路无烟煤的微晶结构,晶粒尺寸增加,平均芳香层数可达54.84,有利于后续氧化插层形成氧化石墨烯;氧化反应产生了大量含氧官能团,增加了煤基氧化石墨烯的缺陷度(ID1/IG=2.06),层间距可达0.790 nm;还原氧化石墨烯表面含氧官能团大幅度减少,缺陷度减小至1.58,芳构碳的有序度增加,成功制得煤基石墨烯;透射电镜下发现小发路无烟煤晶格条纹大部分为无定向弯曲,层间堆垛较厚,所制备的煤基石墨烯则呈透明薄层状,表面含有较多翘曲,边缘处可观察到线性晶格条纹,层数达3~5层。小发路无烟煤的含氧官能团以酚、醇、醚、酯为主,羧基含量较低,羟基共检测到环状羟基、与醚作用形成氢键的羟基、羟基间氢键相连的羟基、与芳香体系形成氢键的羟基以及自由羟基等5种,氧化后的煤基氧化石墨烯表面含氧官能团以醚和/或环氧化物、自缔合羟基和OH—醚氧键/环状羟基和羧基为主,而还原后煤基石墨烯中剩余的少量含氧官能团主要为醚和/或环氧化物,其稳定性较强,通过水合肼还原难以消除。

     

    Abstract: In order to study the preparation and spectroscopic characterization of coal-based graphene from an-thracite in Xiaofalu,a coal-based graphene was prepared by modified Hummers redox method,and the chemical structures of raw coal and process products were characterized by transmission electron microscope ( TEM), X-ray diffraction (XRD),Raman spectrum and Fourier transform infrared spectroscopy ( FT-IR). The results show that high tempera- ture graphitization significantly improves the microcrystalline structure of Xiaofalu anthracite,in-creases the crystallite size,and the average aromatic layer number can reach 54. 84,which is conducive to the formation of graphene oxide. The oxidation reaction produces a large number of oxygen functional groups,which increases the defect degree of coal- based graphene oxide (ID1 / IG = 2. 06),and the layer spacing is up to 0. 790 nm. The oxygen functional groups on the surface of graphene are greatly reduced,the defect degree decreases to 1. 58,and the order degree of aromatic carbon increases,the coal-based graphene is successfully obtained. Under the transmission electron microscopy,it is found that the lattice fringes of Xiaofalu anthracite coal are mostly non-directionally curved,and the stacking between layers is thicker. The coal-based graphene has a transparent thin layer,and the surface contains more warpage. Linear lattice stripes can be observed at the edges,and the number of layers reaches 3 to 5 layers. The oxygen-containing functional groups of Xiaofalu anthracite are mainly phenol,alcohol,ether and ester. Five kinds of hydroxyl groups are detected. The oxygen functional groups on the surface of coal-based graphene oxide are ether and / or epoxide,self-associated hy- droxyl group and OH—ether bond / cyclic hydroxyl group is dominant,and the remaining small amount of oxygen-con- taining functional groups in the coal-based graphene after reduction is mainly ether and / or epoxide,which is stable and difficult to be eliminated.

     

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