Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 164, Issue -, Pages 204-216Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2014.09.010
Keywords
Direct hydrodesulfurization; Nickel iron phosphides; 4,6-Dimethyldibenzothiophene; FTIR; EXAFS
Funding
- US Department of Energy, Office of Basic Energy Sciences [DE-FG02-96ER14669]
- Humboldt Foundation
- Deutsche Forschungsgemeinschaft (Cluster of Excellence Unifying Concepts in Catalysis)
- Grants-in-Aid for Scientific Research [26289301] Funding Source: KAKEN
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A series of NiFeP/SiO2 catalysts with different Ni:Fe molar ratios (1:0,3:1, 1:1, 1:3,0:1) was investigated for the hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene. The Fe component is a good probe for active sites because Ni2P and Fe2P adopt the same hexagonal crystal structure, yet Fe2P is completely inactive for HDS. X-ray diffraction analysis and FTIR spectroscopy of adsorbed CO indicated the formation homologous alloys. At 3.1 MPa and 613 K (340 degrees C) the activity of the alloys was similar to that of Ni2P, which was very high. There was also unprecedented selectivity toward direct desulfurization (DDS). A reconstruction of the NiFe phase occurred to expose more Ni sites, likely driven by the formation of surface Ni-S bonds as observed by EXAFS. The analysis showed that Ni(2) pyramidal sites responsible for hydrogenation were largely replaced by Fe. This left behind Ni(1) tetrahedral sites which favor DDS and explains the reactivity results. (C) 2014 Elsevier B.V. All rights reserved.
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