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基于临氢热解反应研究石油沥青质中镍和钒化合物的存在形态

郑方 王艳斌 霍达 王春燕 曹青 何京 史权

郑方, 王艳斌, 霍达, 王春燕, 曹青, 何京, 史权. 基于临氢热解反应研究石油沥青质中镍和钒化合物的存在形态[J]. 燃料化学学报. doi: 10.1016/S1872-5813(23)60333-0
引用本文: 郑方, 王艳斌, 霍达, 王春燕, 曹青, 何京, 史权. 基于临氢热解反应研究石油沥青质中镍和钒化合物的存在形态[J]. 燃料化学学报. doi: 10.1016/S1872-5813(23)60333-0
ZHENG Fang, WANG Yan-bin, HUO Da, WANG Chun-yan, CAO Qing, HE Jing, SHI Quan. Morphology study of nickel and vanadium in asphaltene via hydropyrolysis[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(23)60333-0
Citation: ZHENG Fang, WANG Yan-bin, HUO Da, WANG Chun-yan, CAO Qing, HE Jing, SHI Quan. Morphology study of nickel and vanadium in asphaltene via hydropyrolysis[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(23)60333-0

基于临氢热解反应研究石油沥青质中镍和钒化合物的存在形态

doi: 10.1016/S1872-5813(23)60333-0
详细信息
    通讯作者:

    E-mail: zhengfang010@petrochina.com.cn

    wangyanbin1@petrochina.com.cn

  • 中图分类号: TE622

Morphology study of nickel and vanadium in asphaltene via hydropyrolysis

  • 摘要: 石油中的镍、钒化合物主要分布在沥青质中,由于沥青质组成的复杂性,镍和钒化合物的存在形态很难直接得到有效表征。本文通过临氢热解方法处理委内瑞拉减压渣油沥青质,通过电感偶合等离子体质谱仪(ICP MS)、紫外-可见光光谱仪(UV-Vis)、高温气相色谱-原子发射检测器联用仪(HT GC-AED)和傅立叶离子回旋共振质谱(FT-ICR MS)等手段分析表征反应产物,探究沥青质的分子组成与结构,以及镍和钒化合物的存在形态。实验结果表明,随着临氢热解反应温度从330 ℃升高至410 ℃,反应产物的甲苯可溶物收率由64%下降至19%,可被GC-AED检测到的镍、钒化合物的含量大幅度升高,镍和钒卟啉的分子组成分布也随反应温度的升高呈现出规律性的变化。
  • 图  1  沥青质临氢热解处理后各样品UV-vis谱图及局部放大图

    Figure  1  UV-vis spectra of these hydropyrolysis treated asphaltenes derived from Venezuela VR

    图  2  委内瑞拉减渣C7沥青质临氢热解实验处理后各样品的高温GC-AED谱图(钒和镍元素)

    Figure  2  High temperature GC-AED chromatograms of the hydropyrolysis treated asphaltenes derived from Venezuela VR (V and Ni elements)

    图  3  沥青质临氢热解产物中N4VO类化合物的DBE与碳数分布图,图中给出了C30H31N4O1V1 和 C36H31N4O1V1钒卟啉的可能结构

    Figure  3  Relative ion abundance plots of DBE versus carbon number of N4VO class species assigned from positive-ion ESI FT-ICR mass spectra the hydropyrolysis treated asphaltenes derived from the Venezuela VR. The proposed structure of C30H31N4O1V1 and C36H31N4O1V1 are shown based on the molecular composition

    表  1  委内瑞拉重油减渣组分C7沥青质临氢热解反应后甲苯可溶物收率

    Table  1  Toluene soluble yields of hydropyrolysis products derived from the asphaltenes of Venezuelan VR

    Sample0#
    CG
    1#
    330 ℃
    2#
    350 ℃
    3#
    370 ℃
    4#
    390 ℃
    5#
    410 ℃
    Yield(wt%)986460514519
    下载: 导出CSV

    表  2  沥青质临氢热解反应后甲苯可溶物中镍和钒含量

    Table  2  Nickel and vanadium contents of hydropyrolysis products derived from the asphaltenes of Venezuelan VR

    Sample0#
    CG
    1#
    330 ℃
    2#
    350 ℃
    3#
    370 ℃
    4#
    390 ℃
    5#
    410 ℃
    V(μg/g189616401400147316091305
    Ni(μg/g439400412404441310
    下载: 导出CSV

    表  3  委内瑞拉减渣C7沥青质临氢热解后各样品中镍、钒元素的GC-AED信号丰度与对照组的比率

    Table  3  The signal peak area ratio of nickel and vanadium in reaction group and control group detect by GC-AED.

    Sample0#
    CG
    1#
    330 ℃
    2#
    350 ℃
    3#
    370 ℃
    4#
    390 ℃
    5#
    410 ℃
    V(ratio)1.00.90.91.01.13.6
    Ni(ratio)1.01.01.31.93.814.4
    下载: 导出CSV
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出版历程
  • 收稿日期:  2022-12-09
  • 录用日期:  2022-12-27
  • 修回日期:  2022-12-25
  • 网络出版日期:  2023-01-10

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