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负载型加氢脱硫催化剂的声化学制备

Sonochemical preparation of supported hydrodesulfurization catalysts.

作者信息

Dhas N A, Ekhtiarzadeh A, Suslick K S

机构信息

School of Chemical Sciences, University of Illinois at Urbana-Champaign, 600 South, Mathews Avenue, Urbana, IL 61801, USA.

出版信息

J Am Chem Soc. 2001 Aug 29;123(34):8310-6. doi: 10.1021/ja010516y.

DOI:10.1021/ja010516y
PMID:11516280
Abstract

Sonochemical preparation of Co and Ni promoted MoS(2) supported on alumina was achieved by high-intensity ultrasonic irradiation of isodurene solutions containing molybdenum carbonyl, dicobalt octacarbonyl, elemental sulfur, and Al(2)O(3) or Ni-Al(2)O(3) under Ar flow. The sonochemically prepared catalysts were characterized by elemental analysis, XPS, SEM, TEM, and XEDS, and hydrodesulfurization (HDS) activity evaluated for thiophene and dibenzothiophene substrates. The TEM studies on the sonochemically prepared catalysts indicate the formation of layered hexagonal MoS(2) (lattice fringes approximately 6.2 A) on the alumina support. The sonochemically prepared Co-Mo-S/Al(2)O(3), Ni-Mo-S/Al(2)O(3), and Co-Ni-Mo-S/Al(2)O(3) are extremely active catalysts for the HDS of thiophene and dibenzothiophene, with activities severalfold those of comparable commercial catalysts under identical conditions. The layered structure of MoS(2) remained intact after 120 h of HDS, and the catalyst is reusable.

摘要

通过在氩气流下对含有羰基钼、八羰基二钴、单质硫以及氧化铝或镍 - 氧化铝的均三甲苯溶液进行高强度超声辐照,实现了在氧化铝上负载的钴和镍促进的二硫化钼的声化学制备。通过元素分析、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和能量散射X射线谱(XEDS)对声化学制备的催化剂进行了表征,并对噻吩和二苯并噻吩底物评估了加氢脱硫(HDS)活性。对声化学制备的催化剂的TEM研究表明在氧化铝载体上形成了层状六方二硫化钼(晶格条纹约为6.2埃)。声化学制备的Co - Mo - S/Al₂O₃、Ni - Mo - S/Al₂O₃和Co - Ni - Mo - S/Al₂O₃是用于噻吩和二苯并噻吩加氢脱硫的极具活性的催化剂,在相同条件下其活性是可比商业催化剂的几倍。在加氢脱硫120小时后,二硫化钼的层状结构保持完整,并且该催化剂可重复使用。

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