石油炼制与化工 ›› 2018, Vol. 49 ›› Issue (11): 60-65.

• 基础研究 • 上一篇    下一篇

Mo/γ-Al2O3催化剂中金属-载体相互作用位点的研究

户安鹏,李明丰,韩伟,张乐,龙湘云,聂红   

  1. 中国石化石油化工科学研究院
  • 收稿日期:2018-04-09 修回日期:2018-04-26 出版日期:2018-11-12 发布日期:2018-11-29
  • 通讯作者: 聂红 E-mail:niehong.ripp@sinoepc.com
  • 基金资助:
    国家重点研发计划项目

STUDY ON METAL-SUPPORT INTERACTION SITES OVER Mo/γ-Al2O3 CATALYSTS

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  • Received:2018-04-09 Revised:2018-04-26 Online:2018-11-12 Published:2018-11-29
  • Contact: Nie Hong E-mail:niehong.ripp@sinoepc.com
  • Supported by:
     

摘要: 载体表面性质直接影响金属-载体相互作用的强弱,进而对加氢催化剂的结构和性能产生重要影响。为深入认识载体表面性质对金属-载体相互作用的影响机制,以工业加氢催化剂RS-2100的载体为研究对象,首先通过对其进行不同温度(20~180 ℃)的水热处理,调变了其表面各种位点(碱性、中性、酸性羟基及Al-CUS)的相对浓度,然后借助IR-OH和Py-IR表征手段对这些位点相对浓度的变化进行了分析,并采用Mo平衡吸附法对金属-载体相互作用强弱进行了量化分析。IR-OH和Py-IR分析结果表明,随水热处理温度的升高,载体表面碱性羟基和酸性羟基的浓度均先增加后减少,且均在100 ℃水热处理时浓度最大,但后者的浓度在水热处理温度大于100 ℃时减少幅度较小;中性羟基浓度和Al-CUS浓度则随水热处理温度的升高逐渐降低。Mo平衡吸附量分析结果表明,随水热处理温度的升高,金属-载体相互作用先增强后减弱。对上述两方面结果进行关联可以推测,碱性羟基是Mo金属-载体相互作用的关键位点。

关键词: Mo/γ-Al2O3, 水热温度, 金属-载体相互作用, 平衡吸附量, 作用位点

Abstract: Metal-support interaction imposes a great influence on the structure and catalytic activity of the hydrogenation catalysts, and meanwhile it directly depends on the surface properties of the support. In this article, for deeply understanding the influencing mechanism of the support properties on the interaction, the support used for industrial RS-2100 catalyst was first hydrothermally treated under different temperatures (from 20 ℃ to 180 ℃) and the relative concentration of sites on support surface (including basic hydroxyl groups, neutral hydroxyl groups, acidic hydroxyl groups and coordinatively unsaturated sites) were modified. The obtained samples were then characterized by IR-OH and Py-IR, and the strength of metal-support interaction was evaluated according to the equilibrium adsorption contents of MoO3 on the support surface. IR-OH and Py-IR analysis results indicate that, with the increase of the hydrothermal temperature, the relative concentration of either basic hydroxyl groups or acidic hydroxyl groups first increases and then decreases, and reaches the maximum at 100 ℃. While the relative concentration of acidic hydroxyl groups decreases slightly after 100 ℃, and whereas that of either the neutral hydroxyl groups or Al-CUS gradually decreases. Meanwhile, according to the results of equilibrium adsorption contents of MoO3, it can be seen that, with the increase of temperature, the metal-support interaction first increases and then decreases. Based on the above analysis results, the suggestion that the metal-support interaction is mainly originated from the basic hydroxyl groups on the alumina surface can be given.

Key words: Mo/γ-Al2O3, hydrothermal temperature, metal-support interaction, equilibrium adsorption site, interaction site

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