Microstructural analysis of nitrogen-doped char by Raman spectroscopy: Raman shift analysis from first principles
Microstructural analysis of nitrogen-doped char by Raman spectroscopy: Raman shift analysis from first principles
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DOI：
10.1016/j.carbon.2020.05.055
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发表时间：
2020-10-15
期刊：
影响因子：
10.9
通讯作者：
Garcia-Perez, Manuel
中科院分区：
文献类型：
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作者：
Ayiania, Michael;Weiss-Hortala, Elsa;Garcia-Perez, Manuel
氮掺杂材料具有独特的功能性质，使其在环境、多相催化和电子领域具有潜在的应用价值。为了更好地理解这些官能团对焦拉曼光谱的影响，我们构建了各种含N官能团的多芳香族结构的第一性原理模型。N个官能团的存在在1400-1550 cM(-1)和1605-1650 cM(-1)之间引起了活跃的振动。我们利用这些见解来说明使用纤维素/三聚氰胺混合物2：1在350℃到700℃之间产生的N掺杂纤维素焦的去卷积。随着温度的升高，D带和G带的强度一致地增加，这与芳香族簇的大小有关。当碳化温度从350℃升高到700℃时，A带(谷区)的持续减少与杂原子(主要是N和O)的损失有关。虽然本文中报道的模拟结果用于通知N掺杂碳拉曼光谱的反卷积，但它们也与其他纳米碳基材料的研究相关。(C)2020爱思唯尔有限公司。保留所有权利。
Nitrogen-doped materials are known to possess unique functional properties, making these materials potentially useful for environmental applications, heterogeneous catalysis, and electronics. In this paper we constructed first principles-based models of various polyaromatic structures containing N functionalities to better understand the effect of these functional groups on char Raman spectra. The presence of N functional groups induces active vibrations in the regions between 1400 and 1550 cm(-1) and 1605-1650 cm(-1). We used these insights to inform the deconvolution of N-doped cellulose char produced between 350 and 700 degrees C using cellulose/melamine blends 2:1. A consistent increase in the intensity of the D and G bands is observed with temperature, which is related to an increase in size of the aromatic cluster. A consistent decrease in the A (the valley region) band is related to the loss of heteroatoms (mainly N and O) as the carbonization temperature increases from 350 to 700 degrees C. Although the modeling results reported in this manuscript are used to inform the deconvolution of N-doped char Raman spectra, they are also relevant to study other nanocarbon-based materials. (C) 2020 Elsevier Ltd. All rights reserved.