Unsupported NiMoAl hydrotreating catalysts prepared from NiAl-terephthalate hydrotalcites exchanged with heptamolybdate

被引:14
作者
Arias, Santiago [1 ]
Licea, Yordy E. [1 ]
Palacio, Luz Amparo [2 ]
Faro, Arnaldo C., Jr. [1 ]
机构
[1] Univ Fed Rio de Janeiro, Inst Quim, BR-21941909 Rio De Janeiro, Brazil
[2] Univ Estado Rio de Janeiro, Inst Quim, BR-20550900 Rio De Janeiro, Brazil
关键词
NiMo; Unsupported catalysts; HDS; HDA; Terephthalate; Layered double hydroxide; LAYERED DOUBLE HYDROXIDES; SULFIDE CATALYSTS; MIXED OXIDES; HYDRODESULFURIZATION; ADSORPTION; 4,6-DIMETHYLDIBENZOTHIOPHENE; DIBENZOTHIOPHENES; THIOPHENE; OXIDATION; TEXTURE;
D O I
10.1016/j.cattod.2013.02.029
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Unsupported NiMoAl hydrotreating catalysts were prepared starting from NiAl-terephthalate layered double hydroxides (LDHs) with x values (Al/(Al + Ni) ratios) in the 0.3-0.8 range by ion exchange with ammonium heptamolybdate, followed by calcination at 723 K. Mixed oxides containing ca. 33-43 wt% molybdenum and Ni/Mo atomic ratios in the 0.5-1.4 range were obtained. There was loss in the long-range ordering of the LDHs in the c direction during the ion-exchange, but the local structure of the brucite layers was maintained. The calcined mixed-oxides had surface areas ranging from 26 to 122 m(2) g(-1). The catalysts were sulphided in situ and subsequently tested in the simultaneous dibenzothiophene (DBT) HDS and tetralin (THN) hydrogenation reactions in a high pressure batch reactor at 613 K and 70 bar. The catalysts had higher specific activity for both the HDS and the HDA reactions and much higher selectivity for the ring hydrogenation (HYD) route in the HDS of DBT than a conventional NiMo/Al2O3 catalyst. Their activities in both reactions were similar to those of an Al-free unsupported NiMo catalyst, but their preference for the HYD route was higher than that of the latter. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:198 / 205
页数:8
相关论文
共 41 条
[31]   Alumina-, niobia-, and niobia/alumina-supported NiMoS catalysts:: Surface properties and activities in the hydrodesulfurization of thiophene and hydrodenitrogenation of 2,6-dimethylaniline [J].
Rocha, Angela S. ;
Faro, Amaldo C., Jr. ;
Oliviero, Laetitia ;
Van Geste, Jacob ;
Mauge, Francoise .
JOURNAL OF CATALYSIS, 2007, 252 (02) :321-334
[32]   Electronic properties and phase transformations in CoMoO4 and NiMoO4:: XANES and time-resolved synchrotron XRD studies [J].
Rodriguez, JA ;
Chaturvedi, S ;
Hanson, JC ;
Albornoz, A ;
Brito, JL .
JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (08) :1347-1355
[33]   Recent advances in the science and technology of ultra low sulfur diesel (ULSD) production [J].
Stanislaus, Antony ;
Marafi, Abdulazeem ;
Rana, Mohan S. .
CATALYSIS TODAY, 2010, 153 (1-2) :1-68
[34]   The role of reaction pathways and support interactions in the development of high activity hydrotreating catalysts [J].
Topsoe, H ;
Hinnemann, B ;
Norskov, JK ;
Lauritsen, JV ;
Besenbacher, F ;
Hansen, PL ;
Hytoft, G ;
Egeberg, RG ;
Knudsen, KG .
CATALYSIS TODAY, 2005, 107-08 :12-22
[35]   RECENT BASIC RESEARCH IN HYDRODESULFURIZATION CATALYSIS [J].
TOPSOE, H ;
CLAUSEN, BS ;
TOPSOE, NY ;
PEDERSEN, E .
INDUSTRIAL & ENGINEERING CHEMISTRY FUNDAMENTALS, 1986, 25 (01) :25-36
[36]  
Topsoe H., 1996, HYDROTREATING CATALY
[37]   Atomic-scale insight into adsorption of sterically hindered dibenzothiophenes on MoS2 and Co-Mo-S hydrotreating catalysts [J].
Tuxen, Anders K. ;
Fuchtbauer, Henrik G. ;
Temel, Burcin ;
Hinnemann, Berit ;
Topsoe, Henrik ;
Knudsen, Kim G. ;
Besenbacher, Flemming ;
Lauritsen, Jeppe V. .
JOURNAL OF CATALYSIS, 2012, 295 :146-154
[38]   Thermal behavior of oxometalate (Mo,W)-intercalated layered double hydroxides: Study of the grafting phenomenon [J].
Vaysse, C ;
Guerlou-Demourgues, L ;
Demourgues, A ;
Delmas, C .
JOURNAL OF SOLID STATE CHEMISTRY, 2002, 167 (01) :59-72
[39]   THERMAL-PROPERTIES OF TEREPHTHALATE-INTERCALATED AND BENZOATE-INTERCALATED LDH [J].
VUCELIC, M ;
MOGGRIDGE, GD ;
JONES, W .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (20) :8328-8337
[40]   Hydrodesulfurization of 4,6-DMDBT on a multi-metallic sulfide catalyst with layered structure [J].
Wang, Lu ;
Zhang, Yongna ;
Zhang, Yuliang ;
Liu, Peng ;
Han, Hongxian ;
Yang, Min ;
Jiang, Zongxuan ;
Li, Can .
APPLIED CATALYSIS A-GENERAL, 2011, 394 (1-2) :18-24