Abstract
Prof. Doug Ruthven and Prof. Jörg Kärger are two giants in the field of zeolite science and engineering. Over their academic careers encompassing almost forty years each, they have contributed significantly to the advancement of fundamental understanding of adsorption and diffusion in zeolites as well as their industrial applications. The author, in the beginning of his academic career, had an opportunity to spend two years as a post-doctoral fellow in Prof. Ruthven’s laboratory at the University of New Brunswick (1975–1977). This experience actually motivated me to spend my academic career in working in the field of zeolite adsorption and diffusion. Nearly thirty years later, I spent a year as a Gast Mercator Professor at the University of Leipzig in the laboratory of Prof. Kärger (2005–2006). These two opportunities at two different ends of my academic career provided me with unique perspectives to reflect on the important contributions made by Professors Ruthven and Kärger to the field of zeolite science and technology. This article summarizes my personal perspectives on the breadth and depth of their contributions.
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References
Prof. Ruthven’s Papers
Boniface, H.A., Ruthven, D.M.: Use of higher moments to extract transport data from chromatographic adsorption experiments. Chem. Eng. Sci. 40, 2053–2061 (1985)
Boulicaut, L., Brandani, S., Ruthven, D.M.: Liquid phase sorption and diffusion of branched and cyclic hydrocarbons in silicalite. Microporous Mater. 25, 81–93 (1998)
Brandani, S., Ruthven, D.M.: Analysis of ZLC desorption curves for liquid systems. Chem. Eng. Sci. 50, 2055–2059 (1995)
Brandani, F., Ruthven, D.M.: Measurement of adsorption equilibrium by the zero length column (ZLC) technique, part 2: binary systems. Ind. Eng. Chem. Res. 42, 1462–1469 (2003)
Brandani, S., Hufton, J., Ruthven, D.M.: Self diffusion of propane and propylene in 5A and 13X zeolite crystals, studied by tracer ZLC. Zeolites 15, 624–631 (1995)
Brandani, S., Cavalcante, C., Guimaraes, A., Ruthven, D.M.: Heat effects in ZLC experiments. Adsorption 4, 275–285 (1998)
Brandani, S., Jama, M.A., Ruthven, D.M.: ZLC measurements under non-linear conditions. Chem. Eng. Sci. 55, 1205–1212 (2000a)
Brandani, S., Jama, M.A., Ruthven, D.M.: Diffusion, self diffusion and counter-diffusion of benzene and p-xylene in silicalite. Microporous Mesoporous Mater. 35, 283–300 (2000b)
Brandani, F., Ruthven, D.M., Coe, C.G.: Measurement of adsorption equilibrium by the zero length column (ZLC) technique, part 1: single component systems. Ind. Eng. Chem. Res. 42, 1451–1461 (2003)
Ching, C.B., Ruthven, D.M.: Experimental study of a simulated counter-current adsorption system, part I: isothermal, steady state operation. Chem. Eng. Sci. 40, 877–886 (1985a)
Ching, C.B., Ruthven, D.M.: Experimental study of a simulated counter-current adsorption system, part II: transient response. Chem. Eng. Sci. 40, 887–891 (1985b)
Ching, C.B., Ruthven, D.M.: Separation of fructose from glucose by simulated counter-current adsorption. AIChE Symp. Ser. 81(242), 1–8 (1985c)
Ching, C.B., Ruthven, D.M.: Experimental study of a simulated counter-current adsorption system, part IV: nonisothermal operation. Chem. Eng. Sci. 41, 3063–3071 (1986)
Ching, C.B., Ruthven, D.M., Hidajat, K.: Experimental study of a simulated counter-current adsorption system, part III: sorbex operation. Chem. Eng. Sci. 40, 1411–1417 (1985)
Eic, M., Ruthven, D.M.: New experimental technique for measurement of intracrystalline diffusivity. Zeolites 8, 40–45 (1988)
Eic, M., Ruthven, D.M.: Intracrystalline diffusion of linear paraffins and benzene in silicalite studied by the ZLC method. In: Jacobs, P.A., van Santen, R.A. (eds.) Proc. 8th International Zeolite Conf., pp. 897–905. Elsevier, Amsterdam (1989)
Farooq, S., Hassan, M.M., Ruthven, D.M.: Heat effects in pressure swing adsorption systems. Chem. Eng. Sci. 43, 1011–1031 (1988)
Farooq, S., Ruthven, D.M., Boniface, H.A.: Numerical simulation of a PSA oxygen unit. Chem. Eng. Sci. 44, 2809–2816 (1989)
Farooq, S., Ruthven, D.M.: Dynamics of kinetically controlled binary adsorption in a fixed bed. AIChE J. 37, 299–301 (1991)
Garg, D.R., Ruthven, D.M.: On fixed bed sorption of gases with non-linear equilibria. AIChE J. 19, 852–54 (1973)
Garg, D.R., Ruthven, D.M.: Performance of molecular sieve adsorption columns: systems with macropore diffusion control. Chem. Eng. Sci. 29, 1961–1967 (1974a)
Garg, D.R., Ruthven, D.M.: Performance of molecular sieve adsorption columns: systems with micropore diffusion control. Chem. Eng. Sci. 29, 571–581 (1974b)
Garg, D.R., Ruthven, D.M.: Performance of molecular sieve adsorption columns: combined effects of mass transfer and longitudinal diffusion. Chem. Eng. Sci. 30, 1192–1196 (1975)
Haq, N., Ruthven, D.M.: Chromatographic study of sorption and diffusion in 4A zeolite. J. Colloid Interface Sci. 112, 154–163 (1986)
Hassan, M.M., Raghavan, N.S., Ruthven, D.M., Boniface, H.A.: Pressure swing adsorption, part II: experimental study of a linear, isothermal trace component system. AIChE J. 31, 2008–2016 (1985)
Hassan, M.M., Raghavan, N.S., Ruthven, D.M.: Air separation by pressure swing adsorption on a carbon molecular sieve. Chem. Eng. Sci. 41, 1333–1343 (1986)
Hassan, M.M., Raghavan, N.S., Ruthven, D.M.: Numerical simulation of a psa air separation system—comparative study of finite difference and collocation methods. Can. J. Chem. Eng. 65, 512–516 (1987)
Jiang, M., Eic, M., Ruthven, D.M.: Transport properties of ethane, butane and their binary mixtures studied by ZLC. In: Kaneko, K. (ed.) 7th Int. Adsorption Conf. Proceedings, pp. 732–739. IAS (2002)
Raghavan, N.S., Ruthven, D.M.: Pressure swing adsorption, part III: numerical simulation of a kinetically controlled bulk gas separation. AIChE J. 31, 2017–2025 (1985)
Raghavan, N.S., Hassan, M.M., Ruthven, D.M.: Pressure swing adsorption, part I: numerical simulation of an isothermal trace component system. AIChE J. 31, 385–392 (1985)
Risbood, P.A., Ruthven, D.M.: Bromine adsorbed on molecular sieves: a reagent for selective bromination. J. Am. Chem. Soc. 100, 4919–4921 (1978)
Risbood, P.A., Ruthven, D.M.: Selective reduction of aldehydes in presence of ketones. J. Org. Chem. 44, 3969–3970 (1979)
Ruthven, D.M.: A simple theoretical isotherm for zeolites. Nat. Phys. Sci. 232(29), 70–71 (1971)
Ruthven, D.M.: Simple theoretical isotherm for zeolites—further comments. Zeolites 2(4), 242–243 (1982)
Ruthven, D.M., Eic, M., Richard, E.: Diffusion of C8 aromatic hydrocarbons in silicalite. Zeolites 11, 647–653 (1991)
Ruthven, D.M., Farooq, S.: Concentration of a trace component by pressure swing adsorption. Chem. Eng. Sci. 49, 51–60 (1994)
Ruthven, D.M., Kumar, R.: A chromatographic study of diffusion of N2, CH4 and binary CH4-N2 mixtures in 4A molecular sieve. Can. J. Chem. Eng. 57, 342–348 (1979)
Ruthven, D.M., Lee, L.-K.: Nonisothermal sorption kinetics: system with bed diffusion control. AIChE J. 27, 654–663 (1981)
Ruthven, D.M., Garg, D.R., Crawford, R.M.: Performance of molecular sieve adsorption column: nonisothermal systems. Chem. Eng. Sci. 30, 803–810 (1975)
Ruthven, D.M., Tezel, F.H., Devgun, J.S., Sridhar, T.S.: Adsorptive separation of Kr from N2, part I: adsorbent screening studies. Can. J. Chem. Eng. 62, 526–534 (1984)
Ruthven, D.M., Stapleton, P., Dahlke, R.: Application of the ZLC method to measurement of intracrystalline diffusion in liquid-zeolite systems. In: von Ballmoos, R., Higgins, J.B. et al. (eds.) Proc. 9th Int. Zeolite Conf., vol 2, pp. 99–103 (1993)
Shah, D.B., Ruthven, D.M.: Measurement of zeolitic diffusivities and equilibrium isotherms by chromatography. AIChE J. 23, 804–809 (1977)
Tezel, F.H., Ruthven, D.M., Sridhar, T.S.: Development of a chromatographic process for Kr-N2 separation. In: King, C.J. (ed.) Chemical Separation, vol. 2, pp. 339–349. Litarvan Literature, Denver (1986)
Tezel, F.H., Ruthven, D.M., Boniface, H.A., Sridhar, T.S.: Adsorption separation of Kr from N2, II: development of a pilot unit. Can. J. Chem. Eng. 68, 268–277 (1990)
Yoshida, H., Kataoka, T., Ruthven, D.M.: Analytical solution for the breakthrough curve for rectangular isotherm systems. Chem. Eng. Sci. 39, 1489–1497 (1984)
Prof. Ruthven’s Books
Kärger, J., Ruthven, D.M.: Diffusion in Zeolites and Other Microporous Solids. Wiley, New York (1992)
Ruthven, D.M.: Principles of Adsorption and Adsorption Processes. Wiley, New York (1983)
Ruthven, D.M., Farooq, S., Knaebel, K.: Pressure Swing Adsorption. VCH, New York (1993)
Prof. Kärger’s Papers
Appel, M., Fleischer, G., Kärger, J., Fujara, F., Chang, I.: Anomalous segmental diffusion in polymer melts. Macromolecules 27, 4274–4277 (1994)
Bülow, M., Struve, P., Finger, G., Redszus, C., Ehrhardt, K., Schirmer, W., Kärger, J.: Sorption kinetics of n-hexane on MgA zeolites of different crystal size. J. Chem. Soc. Faraday Trans. I 76, 597–615 (1980)
Caro, J., Kärger, J., Finger, G., Pfeifer, H., Schöllner, R.: Zur Selbstdiffusion von Methan und Ethan in A-Zeolithen. Z. Phys. Chem., Leipz. 257, 903–912 (1976)
Caro, J., Bülow, M., Schirmer, W., Kärger, J., Heink, W., Pfeifer, H., Zhdanov, S.P.: Microdynamics of methane, ethane and propane in ZSM-5 type zeolites. J. Chem. Soc. Faraday Trans. I 81, 2541–2550 (1985)
Caro, J., Hocevar, S., Kärger, J., Riekert, L.: Intracrystalline self-diffusion of H2O and CH4 in ZSM-5 zeolites. Zeolites 6, 213–216 (1986)
Chmelik, C., Kärger, J., Wiebcke, M., Caro, J., van Baten, J.M., Krishna, R.: Adsorption and diffusion of alkanes in CuBTC crystals investigated using infra-red microscopy and molecular simulations. Microporous Mesoporous Mater. 117, 22–32 (2009)
Dvoyashkin, M., Valiullin, R., Kärger, J.: Supercritical fluids in mesopores—new insight using NMR. Adsorption 13, 197–200 (2007)
Fleischer, G., Grätz, K., Kärger, J., Mayer, H.W., Quitzsch, K.: Pulsed field gradient nmr self-diffusion study in distinct phases of the ternary system water/n-heptane/igepal CA-520. J. Colloid Interface Sci. 190, 9–16 (1997)
Förste, Ch., Germanus, A., Kärger, J., Pfeifer, H., Caro, J., Pilz, W., Zikanova, A.: Molecular mobility of methane adsorbed on ZSM-5 containing co-adsorbed benzene, and the location of the benzene molecules. J. Chem. Soc. Faraday Trans. I 83, 2301–2309 (1987)
Germanus, A., Kärger, J., Pfeifer, H., Samulevich, N.N., Zhdanov, S.P.: Intracrystalline self-diffusion of benzene, toluene and xylene isomeres in zeolites NaX. Zeolites 5, 91–95 (1985)
Gutsche, R., Fiedler, K., Kärger, J.: Concentration dependence of Fickian diffusivity in solutions and sorption systems. J. Chem. Soc. Faraday Trans. I 81, 3103–3108 (1985)
Hahn, K., Kärger, J., Kukla, V.: Single-file diffusion observation. Phys. Rev. Lett. 76, 2762–2765 (1996)
Heink, W., Kärger, J., Pfeifer, H., Vartapetian, R.S., Voploshchuk, A.M.: PFG NMR study of multicomponent self-diffusion on active carbon. Carbon 31, 1083–1087 (1993)
Heinke, L., Chmelik, C., Kortunov, P., Ruthven, D.M., Shah, D.B., Vasenkov, S., Kärger, J.: Application of interference microscopy and IR microscopy for characterizing and investigating mass transport in nanoporous materials. Chem. Eng. Technol. 30, 995–1002 (2007)
Heyer, W., Janowski, F., Kärger, J., Lenzner, J., Pfeifer, H., Wolf, F.: NMR Untersuchungen zur Desorptionskinetik von Olefin-Paraffin-Gemischen an porösen Gläsern. Z. Chem. 22, 152–153 (1982)
Karge, H.G., Kärger, J.: Application of IR spectroscopy, IR microscopy, and optical interference microscopy to diffusion in zeolites. In: Karge, H.G., Weitkamp, J. (eds.) Adsorption and Diffusion. Molecular Sieves, vol. 7, pp. 135–206. Springer, Berlin (2008)
Kärger, J.: Diffusionsuntersuchung von Wasser an 13X- sowie 4A- und 5A-Zeolithen mit Hilfe der Methode der gepulsten Feldgradienten. Z. Phys. Chem., Leipz. 248, 27 (1971)
Kärger, J.: A straightforward derivation of the long-time limit of the mean square displacement in single-file systems. Phys. Rev. A 45, 4173–4174 (1992)
Kärger, J., Bülow, M.: Theoretical prediction of uptake behaviour in adsorption kinetics of binary gas mixtures using irreversible thermodynamics. Chem. Eng. Sci. 30, 893–896 (1975)
Kärger, J., Caro, J.: Intracrystalline self-diffusion of methane in 5A molecular sieves. J. Colloid Interface Sci. 52, 623–625 (1975)
Kärger, J., Caro, J.: Interpretation and correlation of zeolitic diffusivities obtained from nuclear magnetic resonance and sorption experiments. J. Chem. Soc. Faraday Trans. I 73, 1363–1376 (1977)
Kärger, J., Walter, A.: Messung der Selbstdiffusin von Alkanen an NaX-Zeolithen mit Hilfe der Feldgradientenimpulstechnik der kernmagnetischen Resonanz. Z. Phys. Chem., Leipz. 255, 142–148 (1974)
Kärger, J., Pfeifer, H., Riedel, E., Winkler, H.: Self-diffusion measurements of water adsorbed in NaY zeolites by means of NMR pulsed field gradient techniques. J. Colloid Interface Sci. 44, 187–188 (1973)
Kärger, J., Bülow, M., van Phat, N.: Zur Kinetik der Gasphasenadsorption von n-Hexan an NaX-Zeolith. II. Vergleich der Sorptions- und NMR-Selbstdiffusionsmessungen an Zeolithen von unterschiedlicher Kristallgröße. Z. Phys. Chem., Leipz. 257, 1217–1231 (1976)
Kärger, J., Bülow, M., Lorenz, P.: NMR self-diffusion measurements in n-heptane-benzene mixtures adsorbed on NaX zeolites. J. Colloid Interface Sci. 65, 181–185 (1978a)
Kärger, J., Bülow, M., Struve, P., Kocirik, M., Zikanova, A.: Intercrystalline molecular transport in zeolites studied by uptake experiments and by nuclear magnetic resonance pulsed field gradient techniques. J. Chem. Soc. Faraday Trans. I 74, 1210–1220 (1978b)
Kärger, J., Pfeifer, H., Rauscher, M., Walter, A.: Selbstdiffusion der homologen Reihe der n-Alkane von n-Butan bis n-Oktadekan in NaX-Zeolithen. Z. Phys. Chem., Leipz. 259, 784–790 (1978c)
Kärger, J., Pfeifer, H., Rauscher, M., Walter, A.: Self-diffusion of n-paraffins in NaX zeolite. J. Chem. Soc. Faraday Trans. I 76, 717–737 (1980)
Kärger, J., Pfeifer, H., Rauscher, M., Bülow, M., Samulevich, N.N., Zhdanov, S.P.: Comparative uptake and NMR studies of molecular transport of ethane in 5A zeolites after different sample pretreatment. Z. Phys. Chem., Leipz. 262, 567–576 (1981)
Kärger, J., Krause, W., Pfeifer, H.: Intracrystalline diffusion in ZSM-5 zeolites. Z. Phys. Chem., Leipz. 263, 838–840 (1982)
Kärger, J., Keller, W., Pfeifer, H., Ernst, S., Weitkamp, J.: Unexpectedly low translational mobility of methane and tetrafluoromethane in the large-pore molecular sieve VPI-5. Microporous Mater. 3, 401–408 (1995)
Kärger, J., Kortunov, P., Vasenkov, S., Heinke, L., Shah, D.B., Rakoczy, R.A., Traa, Y., Weitkamp, J.: Unprecedentend insight into diffusion by monitoring the concentration of guest molecules in nanoporous host materials. Angew. Chem., Int. Ed. Engl. 45, 7846–7849 (2006)
Naumov, S., Khokhlov, A., Valiullin, R., Kärger, J., Monson, P.A.: Understanding capillary condensation and hysteresis in porous silicon: network effects within independent pores. Phys. Rev. E 78, 060601(R) (2008)
Nestle, N., Galvosas, P., Zimmermann, C., Stallmach, F., Kärger, J.: Direct investigation of the fate of NAPL contaminations on a hydrating cement matrix by means of magnetic resonance techniques. Environ. Sci. Technol. 38, 880–885 (2004)
Pfeifer, H., Kärger, J., Germanus, A., Schirmer, W., Bülow, M., Caro, J.: Concentration dependence of intracrystalline self-diffusion in zeolites. Adsorption Sci. Tech. Phys. 2, 229–239 (1985)
Roethe, K.-P., Gutsche, R., Richter, W., Roethe, A., Caro, J., Kärger, J.: Adsorption of aromatics on silica gel. Adsorp. Sci. Technol. 3, 65–74 (1986)
Stallmach, F., Gröger, S., Künzel, V., Kärger, J., Yaghi, O.M., Hesse, M., Müller, U.: NMR studies on the diffusion of hydrocarbons on the metal-organic framework material MOF-5. Angew. Chem., Int. Ed. Engl. 45, 2123–2126 (2006)
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Shah, D.B. Doug Ruthven and Jörg Kärger: Their individual and collective contributions to the field of zeolite science and engineering. Adsorption 16, 497–509 (2010). https://doi.org/10.1007/s10450-010-9256-8
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DOI: https://doi.org/10.1007/s10450-010-9256-8