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高温高压水中干酪根热解的拉曼光谱原位研究

In-situ Raman Spectroscopy for Pyrolysis of Kerogen in High Temperature and High Pressure Water

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【作者】 陈晋阳金鹿江程洪斌朱宪

【Author】 CHEN Jin-yang,JIN Lu-jiang,CHENG Hong-bin,ZHU Xian(School of Environmental and Chemical Engineering,Shanghai University,Shanghai 201800,China)

【机构】 上海大学环境与化学工程学院上海大学环境与化学工程学院 上海201800上海201800

【摘要】 利用对顶砧压腔装置,以金刚石作为顶砧,通过观测和采用拉曼光谱对干酪根在高温高压水中热解的具体过程进行了原位研究。由于金刚石顶砧只在约1 332 cm-1波数出现一个很强很尖锐的峰,因此用于压标的石英、介质水以及样品干酪根的拉曼峰都未受影响。测试了在450℃和850 MPa条件下干酪根变化的拉曼峰。随着温度和压力的增加,干酪根在1600 cm-1波数附近由于芳香环振动引起拉曼峰的最大峰位置(mνax)和半高宽(FWHM)存在转折变化。在干酪根热解之前,其芳香环结构和无序结构之间的缺陷向有序化变化。而对于干酪根的热解过程,先是热解为液相碳氢化合物,随后进一步热解为更小分子的成分,如CH4。干酪根的热解过程与压力密切相关,增加压力对热解存在抑制作用。

【Abstract】 The pyrolysis of kerogen in high temperature and high pressure water and its in-situ transformation were studied by Raman spectroscopy using an anvil cell with diamond anvil.Since the diamond anvil exhibited only a very sharp peak at the wavenumber of 1 332 cm-1,the Raman bands of kerogen,quartz and water were easily identified.The variation of Raman spectra of kerogen were measured at this wavenumber up to 450 ℃ and 850 MPa.With the increase of temperature and pressure,the frequency at maximum intensity(νmax) and the full width at half maximum intensity(FWHM) of the band around 1 600 cm-1 of kerogen varied due to the vibration of aromatic ring.Before the pyrolysis of kerogen,the imperfection between the aromatic ring and the random structures varied in an orderly way with increasing temperatures,whereas in the pyrolysis process,kerogen first pyrolyzed to liquid hydrocarbons then further to gaseous hydrocarbons such as CH4.It was found that the pyrolysis was highly related with pressure and that the pyrolysis would be hindered at high pressure.

【基金】 国家自然科学基金资助项目(50578091);上海市重点学科第二期资助项目(T105)
  • 【文献出处】 分析测试学报 ,Journal of Instrumental Analysis , 编辑部邮箱 ,2008年02期
  • 【分类号】X832
  • 【被引频次】6
  • 【下载频次】247
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