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Title: Magnesia-supported nickel catalysts

Abstract

Surface properties and reactivity of Ni/MgO catalysts, air-calcined at temperatures ([Tc]) in the range 400-800[degrees]C, have been evaluated by TEM, IR spectroscopy of adsorbed CO, and catalytic measurements in methane steam reforming. The effects of calcination and reduction temperature on the Ni particle size distribution (PSD) provide evidence of the singular structure properties of the Ni/MgO system. The [open quotes]broad[close quotes] PSD of samples calcined at [Tc] [<=] 600[degrees]C well accounts for the structure model previously described (Arena, F., Horrell, B.A., Cocke, D.L., Parmaliana, A., and Giordano, N., J. Catal. 132, 58 (1991)). IR spectroscopy shows both the formation of mono and polycarbonyls and the occurrence of the CO disproportionation reaction (2CO [rightleftharpoons] CO[sub 2] + C). The higher reactivity towards CO of more dispersed systems has been attributed to the [open quotes]defective nature[close quotes] of small Ni crystallites. Catalytic measurements (Tr = 625[degrees]C; GHSV = 150,000 h[sup -1]) reveal the superior activity of the system calcined at T[sub c] = 400[degrees]C, notwithstanding that a comparable stability for the systems calcined up to 600[degrees]C has been experienced. At higher T[sub c] (>600[degrees]C) the catalytic pattern, both in terms of activity and resistance to coking, is negatively affected by the formationmore » of the [open quotes]bulk[close quotes] NiO-MgO solid solution. The peculiar influence of the mean Ni particle size (20 [<=] d[sub s] [<=] 1400 [angstrom]) on the turnover frequency (TOF, s[sup -1]), resulting in a volcano-shape relationship with the maximum centred at 90-130 [angstrom], has been explained by invoking a structure-sensitive character of the methane stream-reforming reaction on highly dispersed Ni/MgO catalysts. 48 refs., 7 figs., 2 tabs.« less

Authors:
 [1]; ;  [2]; ; ;  [3];  [4]
  1. Universita degli Studi di, Messina (Italy)
  2. Instituto CNR-TAE, Messina (Italy)
  3. Universita degli Studi di, Torino (Italy)
  4. Institute of Catalysis, Novosibirsk (Russian Federation)
Publication Date:
OSTI Identifier:
6153935
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis; (United States)
Additional Journal Information:
Journal Volume: 141:1; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 01 COAL, LIGNITE, AND PEAT; METHANE; STEAM REFORMER PROCESSES; NICKEL COMPOUNDS; CATALYTIC EFFECTS; ABSORPTION SPECTROSCOPY; CALCINATION; CARBON MONOXIDE; CATALYST SUPPORTS; CATALYSTS; HETEROGENEOUS CATALYSIS; MAGNESIUM OXIDES; PARTICLE SIZE; REDUCTION; TEMPERATURE DEPENDENCE; TEMPERATURE RANGE 0400-1000 K; TEMPERATURE RANGE 1000-4000 K; TRANSMISSION ELECTRON MICROSCOPY; ALKALINE EARTH METAL COMPOUNDS; ALKANES; CARBON COMPOUNDS; CARBON OXIDES; CATALYSIS; CHALCOGENIDES; CHEMICAL REACTIONS; DECOMPOSITION; ELECTRON MICROSCOPY; HYDROCARBONS; MAGNESIUM COMPOUNDS; MICROSCOPY; ORGANIC COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; PYROLYSIS; REFORMER PROCESSES; SIZE; SPECTROSCOPY; TEMPERATURE RANGE; THERMOCHEMICAL PROCESSES; TRANSITION ELEMENT COMPOUNDS; 400201* - Chemical & Physicochemical Properties; 010408 - Coal, Lignite, & Peat- C1 Processes- (1987-)

Citation Formats

Parmaliana, A, Arena, F, Frusteri, F, Coluccia, S, Marchese, L, Martra, G, and Chuvilin, A L. Magnesia-supported nickel catalysts. United States: N. p., 1993. Web. doi:10.1006/jcat.1993.1116.
Parmaliana, A, Arena, F, Frusteri, F, Coluccia, S, Marchese, L, Martra, G, & Chuvilin, A L. Magnesia-supported nickel catalysts. United States. doi:10.1006/jcat.1993.1116.
Parmaliana, A, Arena, F, Frusteri, F, Coluccia, S, Marchese, L, Martra, G, and Chuvilin, A L. Sat . "Magnesia-supported nickel catalysts". United States. doi:10.1006/jcat.1993.1116.
@article{osti_6153935,
title = {Magnesia-supported nickel catalysts},
author = {Parmaliana, A and Arena, F and Frusteri, F and Coluccia, S and Marchese, L and Martra, G and Chuvilin, A L},
abstractNote = {Surface properties and reactivity of Ni/MgO catalysts, air-calcined at temperatures ([Tc]) in the range 400-800[degrees]C, have been evaluated by TEM, IR spectroscopy of adsorbed CO, and catalytic measurements in methane steam reforming. The effects of calcination and reduction temperature on the Ni particle size distribution (PSD) provide evidence of the singular structure properties of the Ni/MgO system. The [open quotes]broad[close quotes] PSD of samples calcined at [Tc] [<=] 600[degrees]C well accounts for the structure model previously described (Arena, F., Horrell, B.A., Cocke, D.L., Parmaliana, A., and Giordano, N., J. Catal. 132, 58 (1991)). IR spectroscopy shows both the formation of mono and polycarbonyls and the occurrence of the CO disproportionation reaction (2CO [rightleftharpoons] CO[sub 2] + C). The higher reactivity towards CO of more dispersed systems has been attributed to the [open quotes]defective nature[close quotes] of small Ni crystallites. Catalytic measurements (Tr = 625[degrees]C; GHSV = 150,000 h[sup -1]) reveal the superior activity of the system calcined at T[sub c] = 400[degrees]C, notwithstanding that a comparable stability for the systems calcined up to 600[degrees]C has been experienced. At higher T[sub c] (>600[degrees]C) the catalytic pattern, both in terms of activity and resistance to coking, is negatively affected by the formation of the [open quotes]bulk[close quotes] NiO-MgO solid solution. The peculiar influence of the mean Ni particle size (20 [<=] d[sub s] [<=] 1400 [angstrom]) on the turnover frequency (TOF, s[sup -1]), resulting in a volcano-shape relationship with the maximum centred at 90-130 [angstrom], has been explained by invoking a structure-sensitive character of the methane stream-reforming reaction on highly dispersed Ni/MgO catalysts. 48 refs., 7 figs., 2 tabs.},
doi = {10.1006/jcat.1993.1116},
journal = {Journal of Catalysis; (United States)},
issn = {0021-9517},
number = ,
volume = 141:1,
place = {United States},
year = {1993},
month = {5}
}