煤焦油的拉曼光谱表征和组分识别

余立旺; 尤静林; 王媛媛; LU Li-ming; 解迎芳; 柳晓飞; 伏清

煤焦油的拉曼光谱表征和组分识别

1.
上海大学省部共建高品质特殊钢冶金与制备国家重点实验室, 上海 200072;
2.
CSIRO Process Science and Engineering, Kenmore, QLD4069, Australia

基金项目: 国家自然科学基金(50932005, 20973107, 40973046); 上海市科委科技基金(12520709200); 澳大利亚CSIRO Minerals Down Under Flagship基金资助。

详细信息

通讯作者:
尤静林,E-mail: jlyou@staff.shu.edu.cn。

中图分类号: O657.37
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- 文章访问数: 602
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- 被引次数: 0
出版历程
- 收稿日期: 2014-09-01
- 刊出日期: 2015-05-30

Characterization of coal tar and components identification by Raman spectroscopy

1.
Shanghai Key Laboratory of Advanced Special Steel, Shanghai University, Shanghai 200072, China;
2.
CSIRO Process Science and Engineering, Kenmore, QLD4069, Australia

摘要

摘要: 用355 nm激光作为激发光源检测了煤焦油常温拉曼光谱;应用两种量子化学计算程序(Gaussian-DFT和ADF)模拟了占总量1%以上的15种煤焦油组分的拉曼光谱,模拟结果与实验光谱能较好匹配,并对振动模式进行了归属分析。研究表明,煤焦油组分主要由共轭六元环构成,其拉曼光谱特征谱带主要在1 660、1 420和1 265 cm^-1附近,当共轭六元环成链式结构时,1 420 cm^-1谱带特征明显;五元环嵌入共轭六元环链式结构会导致其拉曼光谱在1 265和1 660 cm^-1谱带相对强度增大;五元环、杂原子基团和甲基侧链依附在共轭六元环上,则对组分的拉曼光谱影响不显著。
- 拉曼光谱 /
- 煤焦油 /
- 量子化学计算
Abstract: Raman spectrum of coal tar was measured by using 355 nm laser at ambient temperature. Simultaneously, Raman spectra of 15 components which each weighted more than 1% in coal tar were also simulated. The calculated results are in good agreement with the experimental ones and the vibrations of Raman spectra of coal tar are assigned. The results indicate that the most components of coal tar are mainly composed of six-membered ring type hydrocarbons with the characteristic bands at 1 660, 1 420 and 1 265 cm^-1, which are attributed to the C-C stretching vibrations. When the hydrocarbons connect each other in a resonant mode and chain-like structure, 1 420 cm^-1 band is demonstrated significantly. When the hydrocarbons are embedded by the five-member ring type hydrocarbons, the intensity of 1 265 and 1 660 cm^-1 band increases significantly. There is little effect on the spectra of the component molecule provided the five-membered ring type hydrocarbons, heteroatom groups and methyl are only connected at the edge of the component molecule.
- Raman spectra /
- coal tar /
- quantum chemistry calculation

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参考文献(29)

王柔, 戴服管. 煤焦油及其深加工[J]. 四川化工, 1995, 3: 31-38.(WANG Rou, DAI Fu-guan. Deep processing of coal tar[J]. Sichuan Chem, 1995, 3: 31-38.)

孙鸣, 冯光, 王汝成, 徐龙, 杨艳红, 马晓迅. 陕北中低温煤焦油的分离与GC-MS分析[J]. 石油化工, 2011, 40(6): 667-672.(SUN Ming, FENG Guang, WANG Ru-cheng, XU Long, YANG Yan-hong, MA Xiao-xun. Separation and GC-MS analysis of Shanbei low temperature coal tar[J]. Petro chem Technol, 2011, 40(6): 667-672.)

曲思建, 关北峰, 王艳芳, 陈贵烽. 我国煤温和气化(热解)焦油性质及其加工利用现状与进展[J]. 煤炭转化, 1998, 21(1): 15-20.(QU Si-jian, GUAN Bei-feng, WANG Yan-fang, CHEN Gui-feng. Properties and processing utilization status and development of mild gasification (pyrolysis) tar from coals in China[J]. Coal Convers, 1998, 21(1): 15-20.)

窦红兵, 畅宾平, 郑水山, 马建亮. 煤焦油加工的国内外现状及发展趋势探讨[J]. 河南冶金, 2007, 14(5): 22-23.(DOU Hong-bing, CHANG Bin-ping, ZHENG Shui-shan, MA Jian-liang. Discuss of actuality and development tendency of coal tar processing home and abroad[J]. Henan Metall, 2007, 14(5): 22-23.)

潘孔洲, 叶煌. 国内外煤焦油加工工艺的比较[J]. 燃料与化工, 2002, 33(5): 249-252.(PAN Kong-zhou, YE Huang. Comparison between coal tar processing processes at home and abroad[J]. Fuel Chem Process, 2002, 33(5): 249-252.)

HEROD A A, GEORGE A, ISLAS C A, SUELVES I, KANDIYOTI R. Trace-element partitioning between fractions of coal liquids during column chromatography and solvent separation[J]. Energy Fuels, 2003, 17(4): 862-873.

CASAL M D, CANGA C S, DÍEZ M A, ALVAREZ R, BARRIOCANAL C. Low-temperature pyrolysis of coals with different coking pressure characteristics[J]. J Anal Appl Pyrolysis, 2005, 74(1): 96-103.

NOVOTNY M, STRAND J W, SMITH S L, WIESLER D, SCHWENDE F J. Compositional studies of coal tar by capillary gas chromatographymass spectrometry[J]. Fuel, 1981, 60(3): 213-220.

MCCLENNENA W H, MEUZELAAR H L C, METCALF G S, HILL G R. Characterization of phenols and indanols in coal-derived liquids: Use of Curie-point vaporization gas chromato-graphy/mass spectrometry[J]. Fuel, 1983, 62(12): 1422-1429.

KHANA M A, AHMADA I, ISHAQA M, SHAKIRULLAHA M, JANB M T, REHMANB E, BAHADER A. Spectral characterization of liquefied products of Pakistani coal[J]. Fuel Process Technol, 2004, 85(1): 63-74.

徐秀峰, 张蓬洲, 杨保联, 李丽云, 叶朝辉. 用¹³C-NMR 及 DEPT 技术分析气煤加氢产物中沥青烯段分的组成结构[J]. 燃料化学学报, 1995, 23(4): 410-416.(XU Xiu-feng, ZHANG Peng-zhou, YANG Bao-lian, LI Li-yun, YE Chao-hui. Structural analysis of asphaltenes from hydrogenated PI of gas coal by ¹³C-NMR spectrum and DEPT technique[J]. J Fuel Chem Technol, 1995, 23(4): 410-416.)

MONTES-MORÁNA M A, CRESPOA J L, YOUNG R J, GARCÍA R, MOINELO S R. Mesophase from a coal tar pitch: A Raman spectroscopy study[J]. Fuel Process Technol, 2002, 77: 207-212.

KERSHAW J R, SATHE C, HAYASHI J, LI C Z, CHIBA T. Fluorescence spectroscopic analysis of tars from the pyrolysis of a Victorian brown coal in a wire-mesh reactor[J]. Energy Fuels, 2000, 14(2): 476-482.

韩丽娜, 张荣, 毕继诚. 煤焦油及其组分在超临界水中的反应特性研究[J]. 燃料化学学报, 2009, 36(6): 653-659.(HAN Li-na, ZHANG Rong, BI Ji-cheng. Upgrading of coal tar pitch in supercritical water[J]. J Fuel Chem Technol, 2009, 36(6): 653-659.)

马彩霞, 张荣, 毕继诚. 煤焦油在超临界水中的改质研究[J]. 燃料化学学报, 2003, 31(2): 103-110.(MA Cai-xia, ZHANG Rong, BI Ji-cheng. Upgrading of coal tar in supercritical water[J]. J Fuel Chem Technol, 2003, 31(2): 103-110.)

王连勇, 蔡九菊, 李明杰, 孙华成. 煤焦油热裂解机理研究[J]. 东北大学学报 (自然科学版), 2010, 31(4): 550-554.(WANG Lian-yong, CAI Jiu-ju, LI Ming-jie, SUN Hua-cheng. Study on mechanism of coal tar pyrolysis[J]. J Northeast Univ (Nat Sci), 2010, 31(4): 550-554.)

SHINOHARA H, YAMAKITA Y, OHNO K. Raman spectra of polycyclic aromatic hydrocarbons. Comparison of calculated Raman intensity distributions with observed spectra for naphthalene, anthracene, pyrene, and perylene[J]. J Mol Struct, 1998, 442(1/3): 221-234.

XIN H H, WANG D M, QI X Y, QI G S, DOU G L. Structural characteristics of coal functional groups using quantum chemistry for quantification of infrared spectra[J]. Fuel Process Technol, 2014, 118: 287-295.

MAPELLI C, CASTIGLIONI C, MERONI E, ZERBI G. Graphite and graphitic compounds:Vibrational spectra from oligomers to real materials[J]. J Mol Struct, 1999, 480-481: 615-620.

YOSHIZAWA K, OKAHARA K, SATO T, TANAKA K, YAMABE T. Molecular orbital study of pyrolytic carbons[J]. Carbon, 1994, 32(8): 1517-1522.

YOU J L, JIANG G C, HOU H Y, CHEN H, WU Y Q, XU K D. Quantum chemistry study on superstructure and Raman spectra of binary sodium silicates[J]. J Raman Spectrosc, 2005, 36(3): 237-249.

刘晓伟, 尤静林, 王媛媛, 王晨阳, 刘钦, 王静, 赵婷. Na₃AlF₆-Al₂O₃系熔盐结构的计算模拟与高温拉曼光谱[J]. 中国有色金属学报, 2014, 24(1): 286-292.(LIU Xiao-wei, YOU Jing-lin, WANG Yuan-yuan, WANG Chen-yang, LIU Qin, WANG Jing, ZHAO Ting. Caculations simulation and high temperature Raman spectroscopic on structure of Na₃AlF₆-Al₂O₃ molten salt system[J]. Chin J Nonferrous Met, 2014, 24(1): 286-292.)

柳晓飞, 尤静林, 王媛媛, LU Li-ming, 解迎芳, 余立旺, 伏清. 澳大利亚烟煤热解的拉曼光谱研究[J]. 燃料化学学报, 2014, 42(3): 270-276.(LIU Xiao-fei, YOU Jing-lin, WANG Yuan-yuan, LU Li-ming, XIE Ying-fang, YU Li-wang, FU Qing. Raman spectroscopic studies of Australian bituminous coal pyrolysis[J]. J Fuel Chem Technol, 2014, 42(3): 270-276.)

高晋生. 煤的热解、炼焦和煤焦油加工[M]. 化学工业出版社, 2010.(GAO Jin-sheng. The pyrolysis of coal, metallurgical and coal tar processing[M]. Beijing: Chemical Industry Press, 2010.)

陈敏, 燕慧, 杨文智, 王爱青. 煤焦油主要组分测试方法探析[J]. 煤化工, 2005, 32(5): 39-41.(CHEN Min, YAN Hui, YANG Wen-zhi, WANG Ai-qing. Probe and analysis of the testing method for main components in coal tar[J]. Coal Chem Ind, 2005, 32(5): 39-41.)

MUKAMUREZI G, 谢云飞, 姚卫蓉, 赵冰. 利用密度泛函理论研究六种多环芳烃的分子结构以及拉曼光谱[J]. 光散射学报, 2012, 24(4): 333-338.(MUKAMUREZI G, XIE Yun-fei, YAO Wei-rong, ZHAO Bing. Density functional theory studies on molecular structure and Raman spectroscopy of polycyclic aromatic hydrocarbons[J]. J Light Scattering, 2012, 24(4): 333-338.)

FERRAI A C, ROBERTSON J. Interpretation of Raman spectra of disordered and amorphous carbon[J]. Phys Rev B: Condens Matter Mater Phys, 2000, 61(20): 95-107.

SADEZKY A, MUCKENHUBER H, GROTHE H, NIESSNER R, POSCHL U. Raman microspectroscopy of soot and related carbonaceous materials: Spectral analysis and structural information[J]. Carbon, 2005, 43(8): 1731-1742.

KAWAKAMI M, KARATO T, TAKENAKA T, YOKOYAMA S. Structure analysis of coke, wood charcoal and bamboo charcoal by Raman spectroscopy and their reaction rate with CO₂[J]. ISIJ Int, 2005, 45(7): 1027-1034.

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