Spatially resolved Raman and UV-visible-NIR spectroscopy on the preparation of supported catalyst bodies:: Controlling the formation of H2PMo11CoO405- inside Al2O3 pellets during impregnation

被引:77
作者
Bergwerff, JA
van de Water, LGA
Visser, T
de Peinder, P
Leliveld, BRG
de Jong, KP
Weckhuysen, BM
机构
[1] Univ Utrecht, Debye Inst, Dept Inorgan Chem & Catalysis, NL-3508 TB Utrecht, Netherlands
[2] Albemarle Catalysts BV, NL-1022 AB Amsterdam, Netherlands
关键词
heterometallic complexes; hydrodesulfurization; Raman microscopy; supported catalysts; UV/Vis spectroscopy;
D O I
10.1002/chem.200500116
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The physicochemical processes that occur during the preparation of CoMo-Al2O3, hydrodesulfurization catalyst bodies have been investigated. To this end, the distribution of Mo and Co complexes, after impregnation of gamma-Al2O3 pellets with different CoMoP solutions (i.e., solutions containing Co, Mo, and phosphate), was monitored by Raman and UV-visible-NIR microspectroscopy. From the speciation of the different complexes over the catalyst bodies, insight was obtained into the interaction of the different components in the impregnation solution with the Al2O3 surface. It is shown that. after impregnation with a solution containing H2PMo11CoO405- the reaction of phosphate with the Al2O3 leads to the disintegration of this complex, The consecutive independent transport of Co2+ complexes (fast) and Mo6+ complexes (slow) through the pores of the Al2O3 is envisaged, By the addition of extra phosphate and citrate to the impregnation solution. the formation of the desired heteropolvanion can be achieved inside the pellets. Ultimately, the H2PMo11CoO405- distribution could he controlled by varying the aging time applied after impregnation. the power of it combination of spatially resolved spectroscopic techniques to monitor the preparation of supported catalyst bodies is illustrated.
引用
收藏
页码:4592 / 4601
页数:10
相关论文
共 36 条
[1]   The impact of nanoscience on heterogeneous catalysis [J].
Bell, AT .
SCIENCE, 2003, 299 (5613) :1688-1691
[2]   Envisaging the physicochemical processes during the preparation of supported catalysts:: Raman microscopy on the impregnation of Mo onto Al2O3 extrudates [J].
Bergwerff, JA ;
Visser, T ;
Leliveld, BRG ;
Rossenaar, BD ;
de Jong, KP ;
Weckhuysen, BM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (44) :14548-14556
[3]   Anderson type heteropolyoxomolybdates in catalysis:: 1.: (NH4)3[CoMo6O24H6]•7H2O/γ-Al2O3 as alternative of Co-Mo/γ-Al2O3 hydrotreating catalysts [J].
Cabello, CI ;
Botto, IL ;
Thomas, HJ .
APPLIED CATALYSIS A-GENERAL, 2000, 197 (01) :79-86
[4]   Ligand-promoted alumina dissolution in the preparation of MoOx/gamma-Al2O3 catalysts: Evidence for the formation and deposition of an Anderson-type alumino heteropolymolybdate [J].
Carrier, X ;
Lambert, JF ;
Che, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (42) :10137-10146
[5]   Influence of ageing on MoO3 formation in the preparation of alumina-supported Mo catalysts [J].
Carrier, X ;
Lambert, JF ;
Kuba, S ;
Knözinger, H ;
Che, M .
JOURNAL OF MOLECULAR STRUCTURE, 2003, 656 (1-3) :231-238
[6]   An XAFS study of the different influence of chelating ligands on the HDN and HDS of γ-Al2O3-supported NiMo catalysts [J].
Cattaneo, R ;
Rota, F ;
Prins, R .
JOURNAL OF CATALYSIS, 2001, 199 (02) :318-327
[7]   Correlation between hydrodesulfurization activity and order of Ni and Mo sulfidation in planar silica-supported NiMo catalysts: The influence of chelating agents [J].
Coulier, L ;
de Beer, VHJ ;
van Veen, JAR ;
Niemantsverdriet, JW .
JOURNAL OF CATALYSIS, 2001, 197 (01) :26-33
[8]   MOLYBDENUM(VI) COMPLEX-FORMATION .8. EQUILIBRIA AND THERMODYNAMIC QUANTITIES FOR THE REACTIONS WITH CITRATE [J].
CRUYWAGEN, JJ ;
ROHWER, EA ;
WESSELS, GFS .
POLYHEDRON, 1995, 14 (23-24) :3481-3493
[9]  
de Jong K. P., 1998, CATTECH, V2, P87
[10]   Synthesis of supported catalysts [J].
de Jong, KP .
CURRENT OPINION IN SOLID STATE & MATERIALS SCIENCE, 1999, 4 (01) :55-62