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抗生素菌渣热解特性及氮迁移转化机理研究

杜家兴 李辰旭 周星星 万淦 徐林林 王贲 李德念 孙路石

杜家兴, 李辰旭, 周星星, 万淦, 徐林林, 王贲, 李德念, 孙路石. 抗生素菌渣热解特性及氮迁移转化机理研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2023003
引用本文: 杜家兴, 李辰旭, 周星星, 万淦, 徐林林, 王贲, 李德念, 孙路石. 抗生素菌渣热解特性及氮迁移转化机理研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2023003
DU Jia-xing, LI Chen-xu, ZHOU Xing-xing, WAN Gan, XU Lin-lin, WANG Ben, LI De-nian, SUN Lu-shi. Pyrolysis behavior of antibiotic residues and the mechanism of nitrogen evolution[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023003
Citation: DU Jia-xing, LI Chen-xu, ZHOU Xing-xing, WAN Gan, XU Lin-lin, WANG Ben, LI De-nian, SUN Lu-shi. Pyrolysis behavior of antibiotic residues and the mechanism of nitrogen evolution[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023003

抗生素菌渣热解特性及氮迁移转化机理研究

doi: 10.19906/j.cnki.JFCT.2023003
基金项目: 国家重点研发计划(2019YFC1906605)资助
详细信息
    通讯作者:

    Tel: 027-87545526-8207, E-mail: sunlushi@hust.edu.cn

  • 中图分类号: TK6

Pyrolysis behavior of antibiotic residues and the mechanism of nitrogen evolution

Funds: The project was supported by the National Key R&D Program of China (2019YFC1906605)
  • 摘要: 在固定床上进行了不同温度下(300–700 ℃)青霉素菌渣的热解实验,研究了不同热解温度下三相产物的产率及氮的形态和分布。采用反应分子动力学模拟的方法研究了菌渣中含有的氨基酸(天冬氨酸、组氨酸和谷氨酸)和2, 5-哌嗪二酮(DKP)的热解反应机理。结果表明:随着温度的增加,热解气产率增加,热解焦产率减少,热解油的产率先增加后减少,在500 ℃达到最大为42.3 wt.%。产物中氮含量随温度的变化规律与产率变化趋势一致。相较于H2和烃类气体,CO2和CO更容易在低温下生成。酰胺是热解油中的主要含氮化合物,随着热解温度的增加,其占比逐渐下降。氨基酸的脱氨反应是NH3的主要来源,氨基酸分子间发生脱水环化生成DKP类化合物。DKP热解生成NH3、HCN、HNCO等气体和R-NH、R-NH-R自由基,含氮自由基通过与其它自由基结合或发生环化生成酰胺、酮等化合物存在于热解油和热解焦中。
  • 图  1  青霉素菌渣样品的XPS谱图

    Figure  1  XPS spectrum of penicillin residue samples

    图  2  热解实验装置示意图

    Figure  2  Schematic diagram of the pyrolysis experimental setup

    图  3  优化后的分子模型 (a):天冬氨酸; (b):组氨酸;(c):谷氨酸; (d): DKP

    Figure  3  Molecular models of (a): Aspartic acid; (b): Histidine; (c): Glutamic acid and (d): DKP

    图  4  优化后的三维体系模型 (a):氨基酸; (b): DKP

    Figure  4  Three-dimensional models of reaction systems of (a): Amino acids; (b): DKP

    图  5  不同热解温度下产物的 (a):产率; (b):氮含量

    Figure  5  The (a): yield and (b): nitrogen content of pyrolytic products at different temperatures

    图  6  不同温度下主要气体组分的 (a):体积分数; (b):产率

    Figure  6  The (a): volume fraction and (b): yield of gas components at different temperatures

    图  7  不同温度下热解油中含氮化合物的分布

    Figure  7  The distribution of nitrogen-containing compounds in tar at different temperatures

    图  8  不同温度下氨基酸热解产物随时间的变化

    Figure  8  The evolution of pyrolytic products at different temperatures for amino acids

    图  9  (a):天冬氨酸; (b):组氨酸; (c):谷氨酸的热解反应过程

    Figure  9  The process of pyrolysis reaction of (a): Aspartic acid; (b): Histidine and (c): Glutamic acid

    图  10  DKP热解产物随时间的变化

    Figure  10  The evolution of pyrolytic products for DKP

    图  11  DKP的热解反应过程

    Figure  11  The process of pyrolysis reaction of DKP

    表  1  青霉素菌渣样品工业分析及元素分析(wt.%)

    Table  1  Industrial analysis and elemental analysis of penicillin residue samples (wt.%)

    Industrial analysisElemental analysis
    MoistureAshVolatile matterFixed carbonCHO*NS
    3.7528.3465.502.4130.544.9027.364.780.33
    *差减法
    下载: 导出CSV

    表  2  青霉素菌渣样品中灰分的XRF分析(wt.%)

    Table  2  The XRF analysis of ash in penicillin residue samples (wt.%)

    CompositionCaOSiO2Al2O3P2O5ClK2ONa2OSO3Fe2O3
    Content/%36.2829.5717.776.132.951.991.651.531.52
    下载: 导出CSV
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  • 收稿日期:  2022-10-26
  • 录用日期:  2022-12-30
  • 修回日期:  2022-12-29
  • 网络出版日期:  2023-01-10

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