Fig. 1 Flow diagram of experimental apparatus employed Fig. 2 Porosity change during sulfurization of reduced sample pellets

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Transcription:

Fig. 1 Flow diagram of experimental apparatus employed Fig. 2 Porosity change during sulfurization of reduced sample pellets

Fig. 4 Simultaneous reduction-sulfurization and direct sulfurization of iron oxide pellets, compared with the separate reduction followed by sulfurization Fig. 3 Fig. 5 Ultimate capacities of sample pellets for reduction and sulfurization (a): during reduction of iron oxide pellets (b): during sulfurization of reduced iron pellets Measured weight change of sample pellets (effects of reaction temperature, pellet size and flow rate)

Fig. 6 Measured values of m for reduction and sulfurization Fig. 7 Effect of H2S concentration on the sulfurization rate of reduced sample pellets Fig. 8 Intrinsic reaction rate constants for reduction and sulfurization (obtained from the separate runs), and the comparative sulfurization rate constants of selected metal oxides

Fig. 9 Comparison between reaction rate calculated from Eq. (3) and measured data (reduction) Fig. 10 Comparison between reaction rate calculated from Eq. (3) and measured data (sulfurization) Fig. 11 Comparison of theoretical results with experimental data (effect of intrapellet diffusion of H2S) Fig. 12 Comparison of theoretical results with experimental data (effect of intrapellet diffusion of H2S)

<Subscripts> e = ultimate i = inert P = product R = reactant r = reduction s = sulfurization 0 = initial Nomenclature DG = molecular diffusivity of gas [cm2/sec] dp = diameter of sample pellet [cm] k = reaction rate constant [cm3/mol sec] kf = mass transfer coefficient on the external surface of sample pellet [cm/sec] M = molecular weight [g] m = order of reaction with respect to solid reactant [-] n = order of reaction with respect to gas reactant [-] p= coefficient of effective diffusivity with respect to porosity within sample pellet [-] R = radius of sample pellet [cm] r = radial distance from the center of sample pellet [cm] rg = radius of solid grain [cm] T = absolute temperature [ K] t = reaction temperature [ Ž] W = weight of sample pellet [g] X = conversion of reaction Literature cited 1) Ohtake, T., S. Tone, S. Kimura and T. Morita: Preprint of Autumn Meeting of The Soc. of Chem. Engrs., Japan, No. F-116, Nagoya (1979) 2) Muchi, I. and A. Moriyama: "Yakin Hanno Kogaku", p. 230, Yokendo, Japan (1972) 3) The Chemical Society of Japan: "Kagaku Binran", p. 131, Maruzen, Japan (1966) 4) Tsay, Q. T., W. H. Ray and J. Szekely: AIChE J., 22, 1064 (1976) 5) Wen, C.Y. and M. Ishida: Envi. Sci. & Tech., 7, 703 (1973) 6) Westmoreland, P. R. and D. P. Harrison: Envi. Sci & Tech., 10, 659 (1976) 7) Westmoreland, P. R. and D. P. Harrison: Envi. Sci & Tech., 11, 498 (1977)

Reactivity of Fe2O3 with H2S Contained in Low-Calorie Syngas Masanobu Hasatani, Megumu Yuzawa, Sachio Sugiyama* and C. Y. Wen** Dept. of Chem. Eng., Nagoya Univ., Nagoya 464 For high-temperature direct removal of H2S from low-calorie syngas, the reactivity of an Fe2O3 pellet with hot simulated gas containing H2S was studied by means of TGA (Thermal Gravimetric Analysis) over a temperature range of 600-900 Ž. It has been concluded within the experimental conditions employed that : 1) The weight change during the simultaneous reduction-sulfurization run seems to be derived by simply adding the two curves obtained from reduction and sulfurization respectively. 2) The ultimate conversion of the reduction run is 0.95 }0.05, and at final stage of the sulfurization run the stoichiometric ratio of S to Fe reaches 1.1 }0.1. 3) The values of activation energy are 13.0 and 1.5 kcal/mol for the reduction and sulfurization, respectively. 4) For pellets smaller than 1.1 mm in diameter, the intrinsic reaction rate seems to dominate the overall sulfurization rate. The intrapellet diffusion effect becomes increasingly significant as pellet size increases beyond 1.1 mm. The theoretical over-all sulfurization rate showed fairly good coincidence with the measured rate when the intrapellet diffusivity of H2S was assumed to be second-order with respect to the macro-porosity in the product layer. * Dept. of Appl. Chem., Aichi Inst. of Tech. ** Dept. of Chem. Eng., West Virginia Univ.