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Title: Decomposition of molybdate-hexamethylenetetramine complex: One single source route for different catalytic materials

Abstract

Decomposition of ammonium heptamolybdate-hexamethylentetramine (HMTA) complex (HMTA){sub 2}(NH{sub 4}){sub 4}Mo{sub 7}O{sub 24}.2H{sub 2}O was studied as a function of treatment conditions in the range 300-1173 K. The evolution of solid products during decomposition was studied by thermal analysis and in situ EXAFS. Depending on the nature of the gas used for treatment, single phases of highly dispersed nitrides Mo{sub 2}N, carbide Mo{sub 2}C, or oxide MoO{sub 2} can be obtained. The nature of the products obtained was explained by qualitative thermodynamical considerations. Morphology of the solids considerably depends on such preparation parameters as temperature and mass velocity of the gas flow. For the nitride-based materials, catalytic activity was evaluated in the model thiophene HDS reaction. It was demonstrated that NH{sub 3}-treated samples showed better catalytic activity than N{sub 2}-treated ones due to cleaner surface and better morphology. Transmission microscopy, XRD and XPS studies showed that MoS{sub 2} is formed on the surface during HDS reaction or sulfidation with H{sub 2}S. Optimized nitride-derived catalysts showed mass activity several times higher than unsupported MoS{sub 2} or MoS{sub 2}/Al{sub 2}O{sub 3} reference catalyst. - Graphical Abstract: Depending on the conditions, decomposition of molybdate-HTMA complex yields highly dispersed molybdenum nitride, carbide or oxide. Researchmore » Highlights: > Decomposition of molybdate-HTMA complex yields highly dispersed Mo{sub 2}N, Mo{sub 2}C or MoO{sub 2}. > In situ EXAFS shows formation of common amorphous product MoC{sub x}N{sub y}O{sub z} at 673 K. > Crystalline Mo{sub 2}N with surface area near 200 m{sup 2}/g was obtained at 823 K. > High mass activity in thiophene HDS was observed.« less

Authors:
 [1]; ; ;  [2]; ;  [1];  [1]
  1. Institut de recherches sur la catalyse et l'environnement de Lyon UMR5256, CNRS-Universite de Lyon 1, 2 avenue Albert Einstein, 69626 Villeurbanne cedex (France)
  2. IFP Energies nouvelles, BP 3, 69390 Vernaison (France)
Publication Date:
OSTI Identifier:
21580020
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 184; Journal Issue: 10; Other Information: DOI: 10.1016/j.jssc.2011.08.005; PII: S0022-4596(11)00430-0; Copyright (c) 2011 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION SPECTROSCOPY; ALUMINIUM OXIDES; DECOMPOSITION; FINE STRUCTURE; GAS FLOW; MOLYBDATES; MOLYBDENUM CARBIDES; MOLYBDENUM NITRIDES; MOLYBDENUM OXIDES; MOLYBDENUM SULFIDES; POLYCYCLIC SULFUR HETEROCYCLES; SOLIDS; SURFACE AREA; SURFACES; THERMAL ANALYSIS; THIOPHENE; UROTROPIN; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY; X-RAY SPECTROSCOPY; ALUMINIUM COMPOUNDS; AMINES; CARBIDES; CARBON COMPOUNDS; CHALCOGENIDES; CHEMICAL REACTIONS; COHERENT SCATTERING; DIFFRACTION; ELECTRON SPECTROSCOPY; FLUID FLOW; HETEROCYCLIC COMPOUNDS; MOLYBDENUM COMPOUNDS; NITRIDES; NITROGEN COMPOUNDS; ORGANIC COMPOUNDS; ORGANIC SULFUR COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; PHOTOELECTRON SPECTROSCOPY; PNICTIDES; REFRACTORY METAL COMPOUNDS; SCATTERING; SPECTROSCOPY; SULFIDES; SULFUR COMPOUNDS; SURFACE PROPERTIES; TRANSITION ELEMENT COMPOUNDS

Citation Formats

Chouzier, Sandra, Czeri, Tivadar, Roy-Auberger, Magalie, Pichon, Christophe, Geantet, Christophe, Vrinat, Michel, and Afanasiev, Pavel. Decomposition of molybdate-hexamethylenetetramine complex: One single source route for different catalytic materials. United States: N. p., 2011. Web. doi:10.1016/j.jssc.2011.08.005.
Chouzier, Sandra, Czeri, Tivadar, Roy-Auberger, Magalie, Pichon, Christophe, Geantet, Christophe, Vrinat, Michel, & Afanasiev, Pavel. Decomposition of molybdate-hexamethylenetetramine complex: One single source route for different catalytic materials. United States. doi:10.1016/j.jssc.2011.08.005.
Chouzier, Sandra, Czeri, Tivadar, Roy-Auberger, Magalie, Pichon, Christophe, Geantet, Christophe, Vrinat, Michel, and Afanasiev, Pavel. Sat . "Decomposition of molybdate-hexamethylenetetramine complex: One single source route for different catalytic materials". United States. doi:10.1016/j.jssc.2011.08.005.
@article{osti_21580020,
title = {Decomposition of molybdate-hexamethylenetetramine complex: One single source route for different catalytic materials},
author = {Chouzier, Sandra and Czeri, Tivadar and Roy-Auberger, Magalie and Pichon, Christophe and Geantet, Christophe and Vrinat, Michel and Afanasiev, Pavel},
abstractNote = {Decomposition of ammonium heptamolybdate-hexamethylentetramine (HMTA) complex (HMTA){sub 2}(NH{sub 4}){sub 4}Mo{sub 7}O{sub 24}.2H{sub 2}O was studied as a function of treatment conditions in the range 300-1173 K. The evolution of solid products during decomposition was studied by thermal analysis and in situ EXAFS. Depending on the nature of the gas used for treatment, single phases of highly dispersed nitrides Mo{sub 2}N, carbide Mo{sub 2}C, or oxide MoO{sub 2} can be obtained. The nature of the products obtained was explained by qualitative thermodynamical considerations. Morphology of the solids considerably depends on such preparation parameters as temperature and mass velocity of the gas flow. For the nitride-based materials, catalytic activity was evaluated in the model thiophene HDS reaction. It was demonstrated that NH{sub 3}-treated samples showed better catalytic activity than N{sub 2}-treated ones due to cleaner surface and better morphology. Transmission microscopy, XRD and XPS studies showed that MoS{sub 2} is formed on the surface during HDS reaction or sulfidation with H{sub 2}S. Optimized nitride-derived catalysts showed mass activity several times higher than unsupported MoS{sub 2} or MoS{sub 2}/Al{sub 2}O{sub 3} reference catalyst. - Graphical Abstract: Depending on the conditions, decomposition of molybdate-HTMA complex yields highly dispersed molybdenum nitride, carbide or oxide. Research Highlights: > Decomposition of molybdate-HTMA complex yields highly dispersed Mo{sub 2}N, Mo{sub 2}C or MoO{sub 2}. > In situ EXAFS shows formation of common amorphous product MoC{sub x}N{sub y}O{sub z} at 673 K. > Crystalline Mo{sub 2}N with surface area near 200 m{sup 2}/g was obtained at 823 K. > High mass activity in thiophene HDS was observed.},
doi = {10.1016/j.jssc.2011.08.005},
journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = 10,
volume = 184,
place = {United States},
year = {2011},
month = {10}
}