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Comparison of the sulfiding rate and mechanism of supported NiO and Ni sup 0 particles

Journal Article · · Journal of Catalysis; (United States)
; ;  [1];  [2]
  1. Univ. of Amsterdam (Netherlands)
  2. Unilever Research Lab. Vlaardingen (Netherlands)
The sulfiding rate and mechanism of (I) Al{sub 2}O{sub 3}-supported NiO and (II) Al{sub 2}O{sub 3}-supported Ni{sup 0} particles have been studied using the temperature-programmed sulfiding technique. Both the surface and the core of Ni{sup 0} particles are easier to sulfide than those of NiO particles of comparable size. The Ni{sup 0} surface sulfides at 210 K and the inner layers sulfide between 270 and 500 K; simultaneously with the H{sub 2}S uptake H{sub 2} is produced. The surface layer of NiO and Ni{sup 0} surface species takes place at various temperatures because of differences in the elementary steps involved in H{sub 2}S dissociation. Compared to NiO particles, the surface of Ni{sup 0} particles sulfides at lower temperatures due to a higher dissociation rate of H{sub 2}S on these surfaces. The sulfiding rate of the core of the particles is determined by solid-state diffusion. Sulfiding of the core of the Ni{sup 0} particles is determined by the diffusion rate of the Ni{sup {delta}+} and to a lesser extent by the S{sup {delta}+} and to a lesser extent by the S{sup {delta}{minus}} ions, while sulfiding of the core of the NiO particles is most likely limited by diffusion of the O{sup 2{minus}} ions. Surface nickel sulfide species are relatively more stable than their bulk analogues, possibly due to a relatively high entropy content of surface layers.
OSTI ID:
7141914
Journal Information:
Journal of Catalysis; (United States), Journal Name: Journal of Catalysis; (United States) Vol. 137:1; ISSN 0021-9517; ISSN JCTLA
Country of Publication:
United States
Language:
English