Hydrodenitrogenation of Simple Aromatic Amines on Molybdena Catalysts
TL;DR: In this paper, the authors showed that saturated hydrocarbon as diluent facilitates C N bond hydrogenolysis in the presence of hydrogen, irrespective of the carbon being sp 2 or sp 3 hybridized.
About: This article is published in Applied Catalysis.The article was published on 1989-01-01. It has received 11 citations till now. The article focuses on the topics: Hydrogenolysis & Hydrocarbon.
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TL;DR: In this article, Ni-promoted MoS2 catalysts supported on γ-Al2O3, siliceous SBA-15, and Zr- and Ti-modified Sba-15 were explored for the simultaneous hydrodesulfurization (HDS) of dibenzothiophene (DBT) and hydrodenitrogenation (HDN) of o-propylaniline (OPA).
Abstract: MoS2 and Ni-promoted MoS2 catalysts supported on γ-Al2O3, siliceous SBA-15, and Zr- and Ti-modified SBA-15 were explored for the simultaneous hydrodesulfurization (HDS) of dibenzothiophene (DBT) and hydrodenitrogenation (HDN) of o-propylaniline (OPA). In all cases, OPA reacted preferentially via initial hydrogenation, and DBT was converted through direct sulfur removal. HDN and HDS activities of MoS2 catalysts are determined by the dispersion of the sulfide phase. Ni promotion increased its dispersion and activity for DBT HDS and also increased the rate of HDN via enhancing the rate of hydrogenation. On nonpromoted MoS2 catalysts, HDS was strongly inhibited by NH3, and the addition of Ni dramatically reduced this inhibiting effect. The conclusion is that HDS is proportional to the concentration of Mo and Ni on the edges of sulfide particles. In contrast, the direct hydrodenitrogenation of OPA occurs only on accessible Mo cations and, hence, decreases with increasing Ni substitution. The nature of the supp...
155 citations
TL;DR: In this paper, the influence of the dispersity of the catalysts on their activity is discussed, and data concerning the kinetics and mechanisms of these reactions as well as the possible elementary reactions occurring on the catalyst surface are analyzed.
Abstract: Comparative characteristics of methods for the processing and detoxification of organohalogen waste are described. It is shown that the catalytic hydrogenolysis method is the most promising. Numerous catalytic systems used for hydrogenolysis are examined, the influence of the dispersity of the catalysts on their activity is discussed, and data concerning the kinetics and mechanisms of these reactions as well as the possible elementary reactions occurring on the catalyst surface are analysed. Also discussed are the factors determining the reactivity of the C–Hal bonds in the hydrogenolytic reactions. The bibliography includes 159 references.
62 citations
TL;DR: In this paper, Mo-Ni/Al-SBA-15(10) was used for Methylcyclohexylamine conversion to hydrocarbons and the observed trend of activity is correlated with the aluminum content, and it was concluded that the variation in Si/Al ratio remarkably affects the hydrodenitrogenation ability of Al-Sba-15 supported Mo−Ni catalysts.
Abstract: Mesoporous Al-SBA-15 with different Si/Al molar ratio (10, 20, 30, and 40) was synthesized hydrothermally, and Mo–Ni catalysts were prepared by incipient wet impregnation method and characterized by different techniques. An impressive catalytic performance was observed on Mo–Ni/Al-SBA-15(10) for Methylcyclohexylamine conversion to hydrocarbons. The observed trend of activity is correlated with the aluminum content, and it is concluded that the variation in Si/Al ratio remarkably affects the hydrodenitrogenation ability of Al-SBA-15 supported Mo–Ni catalysts.
52 citations
TL;DR: In this article, the authors show that the presence of Dibenzothiophene (DBT) decreases the DDN rate, while increasing the electron density at the brim sites due to the electron pair donor properties of DBT and biphenyl.
49 citations
TL;DR: The mesoporous molecular sieve, H-AlMCM-41, was synthesized hydrothermally and used as support for the preparation of series of sequentially impregnated NiO-MoO 3 catalysts as discussed by the authors.
Abstract: The mesoporous molecular sieve, H-AlMCM-41 (Si/Al = 100) was synthesized hydrothermally and used as support for the preparation of series of sequentially impregnated NiO-MoO 3 catalysts. Various amounts of MoO 3 (12, 18, 24 and 30 wt.%) along with of 7 wt.% of NiO were loaded in order to optimize the MoO 3 loading level for obtaining maximum HDN activity. These catalysts were well-characterized by physico-chemical techniques, such as X-ray diffraction (XRD), N 2 adsorption–desorption, SEM, FT-Raman spectroscopy, UV–vis DRS and FT-IR spectra of CO adsorption and tested for hydrodenitrogenation (HDN) of o -toluidine. The change in dispersion with MoO 3 loading was studied by FT-IR spectra of CO adsorbed samples. HDN activities of various NiO-MoO 3 catalysts were evaluated and the activities are accounted in terms of physico-chemical characteristics of the catalytic materials. Catalyst with 7 wt.% NiO-24 wt.% MoO 3 showed maximum HDN activity when compared to other catalysts and its enhanced activity due to the fine dispersion of MoO 3 as well as due to formation of an additional Ni–Mo–O phase from AlMCM-41, as revealed by FT-IR of CO adsorption, FT-Raman and XRD studies.
28 citations
References
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TL;DR: The effect of presulfiding of a commercial NiMoAl2O3 catalyst has a significant effect on its inherent activity for the hydrodenitrogenation of quinoline (HDN).
154 citations
TL;DR: Thesis (Ph.D.) as mentioned in this paper, Mass. Institute of Technology, Dept. of Chemical Engineering, 1980, Boston, Massachusetts, United States of America, USA, USA.
Abstract: Thesis (Ph.D.)--Massachusetts Institute of Technology, Dept. of Chemical Engineering, 1980.
106 citations
TL;DR: In this article, the Hofmann degradation chemistry is consistent with the experimental observations reported for HDN reactions in the absence and presence of sulfur, and the role played by H/sub 2/S in the nitrogen removal steps is elucidated.
103 citations
99 citations
TL;DR: In this article, it was shown that indoline and o-ethyl aniline produced in the hydrodenitrogenation of indole inhibits the overall HDN reaction. But, they did not consider the effect of indoline on the subsequent hydrogenolysis of the C N bond of the saturated amine.
44 citations