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1 Studies on the Adsorption Removal of Hydrogen Sulfide Gas Static and dynamic adsorption characteristics of hydrogen sulfide in gaseous phase on porous activated carbons and zeolites Keito Boki Department of Public Health, School of Medicine, Tokushima University, Tokushima The static and dynamic adsorption characteristics of hydrogen sulfide on activated carbons and zeolites were investigated to obtain some fundamental information on the removal of hydrogen sulfide in the gaseous phase. The amount adsorbed and the rate of adsorption were measured by the static method, and the service time was measured by the dynamic method. The adsorption of hydrogen sulfide on adsorbents was expressed by Freundlich's equation at equilibrium concentrations up to 70,000ppm. Among the 24 kinds of adsorbents, the amount adsorbed on activated carbons No.4 and No.8, and zeolites No.16 and No.17 was 36.50, 35.42, 69.23, and 87.55ml/g at 70,000ppm, respectively, and their adsorption attained equilibrium within about ten minutes. It may be concluded that the amount adsorbed on adsorbents was mainly affected by their pore volume in the range of pore radii from 2.2 to 6.5 ð rather than by their chemical properties such as ph, pka, basic amount, and acid amount. The heats of adsorption of Nos. 4, 8, 16, and 17 were less than 18kcal/mol. The amount chemisorbed on the activated carbons and the zeolites was about ten and two %, respectively and, therefore, these adsorbents used seemed to be regenerated by some simple treatment to the extent of the original adsorption capacity. Among the 8 kinds of adsorbents, the service time of No.8 and No.17 (9 `20 mesh) with a concentration of hydrogen sulfide 7,000ppm at a flow rate of the mixed gas (H2S-air) 650ml/cm2 Emin was 23 and 65 minutes, respectively, and no correlation was established between the amount adsorbed and the service time. A linear relationship existed between the service time and the length of column, and the service time was inversely proportional to the flow rate of the mixed gas and the concentration of hydrogen sulfide.

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3 Chart 1 Computer program for calculating pore size distribution A: Bomb (H2S) B: Greaseless valve (Kusano, SM-3) C: Air compressor (Dry air) D1: Float meter (Kusano, FT-1/ ) D2: Float meter (Kusano, FT-1/ ) E: Gas mixer F: Adsorbent G: Thermostat H: Absorbing solution Fig. 1 Apparatus for measuring service time

4 Table 1 Amount of hydrogen sulfide adsorbed on activated carbons Table 2 Amount of hydrogen sulfide adsorbed on zeolites

5 Fig. 2 Effect of temperature on adsorption isotherms of hydrogen sulfide on adsorbents No.4 and No.17 Fig. 3 Application of Freundlich's equation to adsorption isotherms of hydrogen sulfide on several adsorbents

6 Fig. 4 Amount of hydrogen sulfide adsorbed on activated carbons vs. isosteric differential heat of adsorption Fig. 5 Amount of hydrogen sulfide adsorbed on zeolites vs. isosteric differential heat of adsorption

7 Table 3 Fractional approach to equilibrium of hydrogen sulfide on activated carbons and zeolites

8 Table 4 Physicochemical properties of activated carbons and zeolites Table 5 Pore volume of several adsorbents Fig. 6 Pore size distributions of several adsorbents

9 Condition; Concentration of H2S: 7,000ppm Flow rate: 1,000ml/min. (650ml/min cm2) Length of column: 10cm, Diameter of column: 1.4cm.

10 Fig. 7 Effect of column-length on service time Fig. 8 Effect of H2S concentration on service time Fig. 9 Effect of flow rate on service time

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12 12) Dollimore, D. and Heal, G.R.: An Improved Method for the Calculation of Pore Size Distribution from Adsorption Data, J. Appl. Chem., 14, (1964). 14) Hassler, J.W.: Purification with Activated Carbon, p. 266, Chemical Publishing York (1974). Co. Inc., New 15) Deo, A.V., Dalla Lana, I.G. and Habgood, H. W.: Infrared Studies of the Adsorption and Surface Reactions of Hydrogen Sulfide and Sulfur Dioxide on Some Aluminas and Zeolites, J. Cat., 21, (1971). 17) Adamson, A.W.: Physical Chemistry of Surfaces p , , Interscience Publishers, New, York (1967). 18) Tsitsishvili, G.V., Andronikashvili, T. G., Sabelashvili, Sh. d., and Chumburidze, T. A.: In gadsorption-desorption Phenomena h (Editor: F. Ricca), p. 76, Academic Press Inc., London and New York (1972). 20) Dubinin, M.M.: The Potential Theory of Adsorption of Gases and Vapors for Adsorbents with Energetically Nonuniform Surfaces, Chem. Rev., 60, (1966). 21) Dubinin, M.M.: Adsorption in Micropores, J. Colloid Interface Sci., 23, (1967). 22) Dubinin, M.M.: Porous Structure and Adsorption Properties of Active Carbons, Chemistry and Physics of Carbon, 2, (1967). 25) Smith, D.B.A. and Adams, N.G.B.: Adsorption on Solids, p , Butterworth and Co. Ltd., London (1974).

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