Abstract This study describes the use of gel permeation chromatography inductively coupled plasma high-resolution mass spectrometry (GPC ICP HRMS) to examine and explain two important petroleum industry catalytic processes: hydrodemetallization (HDM) and hydrodesulfurization (HDS). The sulfur, nickel and vanadium species size distributions in atmospheric residue fractions were studied to track their evolution during both catalytic processes and examine their mechanisms, especially those mechanisms linked to changes in temperature and initial deactivation via coke laydown. Chromatogram shapes as well as peak areas were used to study the V, Ni and S aggregate types and concentrations in the feedstock as well as in the product after varying the operating temperature and residence time at a constant temperature. For the V and Ni compounds, the low and medium molecular weight (LMW and MMW, respectively) aggregates are easily hydrotreated under all conditions, while the high molecular weight (HMW) compounds are more refractory. For the S compounds, a different reactivity pattern was observed whereby the LMW, MMW and HMW aggregates were more similar in their reactivity, showing that the catalyst is less selective towards a certain aggregate size for the S compounds compared to the V or Ni compounds.

中文翻译：

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了解原油常压渣油加氢脱金属加氢脱硫中V、Ni、S的去除

摘要 本研究描述了使用凝胶渗透色谱电感耦合等离子体高分辨率质谱 (GPC ICP HRMS) 来检查和解释两个重要的石油工业催化过程：加氢脱金属 (HDM) 和加氢脱硫 (HDS)。研究了常压渣油馏分中的硫、镍和钒物种尺寸分布，以跟踪它们在两个催化过程中的演变并检查它们的机制，尤其是那些与温度变化和焦炭沉积初始失活相关的机制。色谱图形状和峰面积用于研究在恒定温度下改变操作温度和停留时间后原料和产品中的 V、Ni 和 S 聚集体类型和浓度。对于 V 和 Ni 化​​合物，低分子量和中等分子量（分别为 LMW 和 MMW）聚集体在所有条件下都易于加氢处理，而高分子量 (HMW) 化合物更难处理。对于 S 化合物，观察到不同的反应模式，其中 LMW、MMW 和 HMW 聚集体的反应性更相似，表明与 V 或 Ni 化​​合物相比，催化剂对 S 化合物的特定聚集体尺寸的选择性较低。