Highly-active nickel phosphide hydrotreating catalysts prepared in situ using nickel hypophosphite precursors

被引:63
作者
d'Aquino, Andrea I. [1 ,2 ]
Danforth, Samuel J. [1 ,2 ]
Clinkingbeard, Tess R. [1 ,2 ]
Ilic, Boris [1 ,2 ]
Pullan, Lee [3 ]
Reynolds, Michael A. [4 ]
Murray, Brendan D. [4 ]
Bussell, Mark E. [1 ,2 ]
机构
[1] Western Washington Univ, Dept Chem, MS 9150,516 High St, Bellingham, WA 98225 USA
[2] Western Washington Univ, Adv Mat Sci & Engn Ctr, Bellingham, WA 98225 USA
[3] FEI Co, 5350 NE Dawson Creek Dr, Hillsboro, OR 97124 USA
[4] Shell Oil Co, Westhollow Technol Ctr, 3333 Highway 6 South, Houston, TX 77082 USA
基金
美国国家科学基金会;
关键词
Hydrodenitrogenation; Carbazole; Hydrodesulfurization; Benzothiophene; Nickel phosphide; Nickel hypophosphite; METAL PHOSPHIDES; THIOPHENE HYDRODESULFURIZATION; HYDROPROCESSING CATALYSTS; LOW-TEMPERATURE; NI2P CATALYSTS; MODEL-COMPOUND; DECOMPOSITION; COBALT; BULK; MOP;
D O I
10.1016/j.jcat.2015.12.006
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
An in situ method for the preparation of nickel phosphide (Ni2P) on silica, alumina, and amorphous silica alumina (ASA) supports is described. The synthesis avoids the use of nickel and phosphorus salts by employing the reaction between nickel hydroxide (Ni(OH)(2)) and hypophosphorus acid (H3PO2), allowing the impregnation of nickel hypophosphite (Ni(H2PO2)(2)) onto the oxide supports in the absence of salt by-products. Temperature-programmed reduction (TPR) in flowing hydrogen at 573-773 K yields phase pure Ni2P on the supports with small average particle sizes (3-4 nm) as measured using transmission electron microscopy. The conversion of Ni(H2PO2)(2) to Ni2P and related reactions were probed using TPR with on-line mass spectral analysis of the gas effluent. Unsupported Ni(H2PO2)(2) reacts in flowing hydrogen to produce PH3 and H2O at 468 and 482 K, respectively; the reaction is shifted to increasingly higher temperatures for Ni(H2PO2)(2) supported on SiO2, Al2O3 and ASA. The hydrodenitrogenation (HDN) and hydrodesulfurization (HDS) properties of the Ni2P catalysts were probed using a mixed feed containing carbazole and benzothiophene. While Ni2P/SiO2 catalysts prepared by the different methods exhibited similar HDN and HDS activities, the in situ prepared Ni2P/Al2O3 and Ni2P/ASA catalysts were substantially more active than their ex situ counterparts prepared from hypophosphite- and phosphate-based precursors. (C) 2015 Elsevier Inc. All rights reserved.
引用
收藏
页码:204 / 214
页数:11
相关论文
共 32 条
[1]   The effect of cobalt addition to bulk MoP and Ni2P catalysts for the hydrodesulfurization of 4,6-dimethyldibenzothiophene [J].
Abu, Ibrahim I. ;
Smith, Kevin J. .
JOURNAL OF CATALYSIS, 2006, 241 (02) :356-366
[2]  
[Anonymous], 2000, JCPDS POWD DIFFR FIL
[3]   Carbazole hydrodenitrogenation over nickel phosphide and Ni-rich bimetallic phosphide catalysts [J].
Bowker, Richard H. ;
Ilic, Boris ;
Carrillo, Bo A. ;
Reynolds, Michael A. ;
Murray, Brendan D. ;
Bussell, Mark E. .
APPLIED CATALYSIS A-GENERAL, 2014, 482 :221-230
[4]   Oxygen-removal of dibenzofuran as a model compound in biomass derived bio-oil on nickel phosphide catalysts: Role of phosphorus [J].
Cecilia, J. A. ;
Infantes-Molina, A. ;
Rodriguez-Castellon, E. ;
Jimenez-Lopez, A. ;
Oyama, S. T. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 136 :140-149
[5]   Dibenzothiophene hydrodesulfurization over cobalt phosphide catalysts prepared through a new synthetic approach: Effect of the support [J].
Cecilia, J. A. ;
Infantes-Molina, A. ;
Rodriguez-Castellon, E. ;
Jimenez-Lopez, A. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 92 (1-2) :100-113
[6]   The Influence of the Support on the Formation of Ni2P Based Catalysts by a New Synthetic Approach. Study of the Catalytic Activity in the Hydrodesulfurization of Dibenzothiophene [J].
Cecilia, J. A. ;
Infantes-Molina, A. ;
Rodriguez-Castellon, E. ;
Jimenez-Lopez, A. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (39) :17032-17044
[7]   A novel method for preparing an active nickel phosphide catalyst for HDS of dibenzothiophene [J].
Cecilia, J. A. ;
Infantes-Molina, A. ;
Rodriguez-Castellon, E. ;
Jimenez-Lopez, A. .
JOURNAL OF CATALYSIS, 2009, 263 (01) :4-15
[8]   A feasible approach to the synthesis of nickel phosphide for hydrodesulfurization [J].
Guan, Qingxin ;
Cheng, Xun ;
Li, Rongguan ;
Li, Wei .
JOURNAL OF CATALYSIS, 2013, 299 :1-9
[9]   A novel synthetic approach to synthesizing bulk and supported metal phosphides [J].
Guan, Qingxin ;
Li, Wei .
JOURNAL OF CATALYSIS, 2010, 271 (02) :413-415
[10]   Alternative synthesis of bulk and supported nickel phosphide from the thermal decomposition of hypophosphites [J].
Guan, Qingxin ;
Li, Wei ;
Zhang, Minghui ;
Tao, Keyi .
JOURNAL OF CATALYSIS, 2009, 263 (01) :1-3