FT-IR study of NO adsorption on MoS2/Al2O3 hydrodesulfurization catalysts: Effect of catalyst preparation

被引:11
作者
van Haandel, L. [1 ]
Hensen, E. J. M. [1 ]
Weber, Th. [1 ]
机构
[1] Eindhoven Univ Technol, Dept Chem Engn & Chem, Schuit Inst Catalysis, Lab Inorgan Mat Chem, De Rondom 70, NL-5612 AP Eindhoven, Netherlands
关键词
Hydrodesulfurization; MoS2; IR spectroscopy; NO adsorption; EXAFS; Active sites; SULFIDE HYDROTREATING CATALYSTS; DENSITY-FUNCTIONAL THEORY; SUPPORTED MOS2 PARTICLES; ATOMIC-SCALE INSIGHT; IN-SITU FTIR; CO ADSORPTION; ACTIVE-SITES; CITRIC-ACID; MORPHOLOGY CHANGE; HAADF-STEM;
D O I
10.1016/j.cattod.2016.07.028
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The effect of catalyst preparation on structure and performance of MoS2/Al2O3 hydrodesulfurization (HDS) catalysts was studied by NO adsorption, monitored by infrared spectroscopy (NO-IR) and complemented with EXAFS. The main bands at 1785 cm(-1) and 1690 cm(-1) were assigned to the v(N-O) stretching vibrations of coupled mono-or dinitrosyl surface complexes. NO adsorption on sulfided catalysts prepared with nitrilotriacetic acid (NTA) or citric acid (CA) gave rise to additional bands in the IR spectra at 1655 cm(-1), 1630 cm(-1) and 1615 cm(-1), assigned to mononitrosyl adsorption modes. Catalysts prepared with NTA and CA were more active in thiophene HDS than calcined or dried catalysts, despite comparable NO uptake (0.10-0.12 NO/Mo). This was attributed to a changed MoS2 edge structure as suggested by the NO-IR data, as well as to an improved degree of sulfidation as observed by EXAFS. Correlating NO uptake with MoS2 dispersion shows that not more than 30-40% of edge and corner sites were probed with NO. This implies that only a small portion of edge sites may act as active sites in HDS catalysis. (C) 2016 Elsevier B.V. All rights reserved
引用
收藏
页码:67 / 73
页数:7
相关论文
共 42 条
[1]   Quantitative Two-Dimensional (2D) Morphology-Selectivity Relationship of CoMoS Nanolayers: A Combined High-Resolution High-Angle Annular Dark Field Scanning Transmission Electron Microscopy (HR HAADF-STEM) and Density Functional Theory (DFT) Study [J].
Baubet, Bertrand ;
Girleanu, Maria ;
Gay, Anne-Sophie ;
Taleb, Anne-Lise ;
Moreaud, Maxime ;
Wahl, Francois ;
Delattre, Veronique ;
Devers, Elodie ;
Hugon, Antoine ;
Ersen, Ovidiu ;
Afanasiev, Pavel ;
Raybaud, Pascal .
ACS CATALYSIS, 2016, 6 (02) :1081-1092
[2]   Recent STM, DFT and HAADF-STEM studies of sulfide-based hydrotreating catalysts: Insight into mechanistic, structural and particle size effects [J].
Besenbacher, F. ;
Brorson, M. ;
Clausen, B. S. ;
Helveg, S. ;
Hinnemann, B. ;
Kibsgaard, J. ;
Lauritsen, J. V. ;
Moses, P. G. ;
Norskov, J. K. ;
Topsoe, H. .
CATALYSIS TODAY, 2008, 130 (01) :86-96
[3]  
CANDIA R, 1984, B SOC CHIM BELG, V93, P763
[4]   Analysis of the role of citric acid in the preparation of highly active HDS catalysts [J].
Castillo-Villalon, Perla ;
Ramirez, Jorge ;
Antonio Vargas-Luciano, J. .
JOURNAL OF CATALYSIS, 2014, 320 :127-136
[5]   Relationship between the hydrodesulfurization of thiophene, dibenzothiophene, and 4,6-dimethyl dibenzothiophene and the local structure of Co in Co-Mo-S sites: Infrared study of adsorbed CO [J].
Castillo-Villalon, Perla ;
Ramirez, Jorge ;
Castaneda, Rocio .
JOURNAL OF CATALYSIS, 2012, 294 :54-62
[6]   How the CO molar extinction coefficient influences the quantification of active sites from CO adsorption followed by IR spectroscopy? A case study on MoS2/Al2O3 catalysts prepared with citric acid [J].
Chen, Jianjun ;
Garcia, Elizabeth Dominguez ;
Oliviero, Laetitia ;
Mauge, Francoise .
JOURNAL OF CATALYSIS, 2015, 332 :77-82
[7]   IR Spectroscopic Evidence for MoS2 Morphology Change with Sulfidation Temperature on MoS2/Al2O3 Catalyst [J].
Chen, Jianjun ;
Labruyere, Vincent ;
Mauge, Francoise ;
Quoineaud, Anne-Agathe ;
Hugon, Antoine ;
Oliviero, Laetitia .
JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (51) :30039-30044
[8]   IR spectroscopy evidence of MoS2 morphology change by citric acid addition on MoS2/Al2O3 catalysts - A step forward to differentiate the reactivity of M-edge and S-edge [J].
Chen, Jianjun ;
Mauge, Francoise ;
El Fallah, Jaafar ;
Oliviero, Laetitia .
JOURNAL OF CATALYSIS, 2014, 320 :170-179
[9]   EXTENDED X-RAY ABSORPTION FINE-STRUCTURE STUDY OF CO-MO HYDRODESULFURIZATION CATALYSTS [J].
CLAUSEN, BS ;
TOPSOE, H ;
CANDIA, R ;
VILLADSEN, J ;
LENGELER, B ;
ALSNIELSEN, J ;
CHRISTENSEN, F .
JOURNAL OF PHYSICAL CHEMISTRY, 1981, 85 (25) :3868-3872
[10]   Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts [J].
Ding, Kunlun ;
Gulec, Ahmet ;
Johnson, Alexis M. ;
Schweitzer, Neil M. ;
Stucky, Galen D. ;
Marks, Laurence D. ;
Stair, Peter C. .
SCIENCE, 2015, 350 (6257) :189-192