CARBON DIOXIDE ON RANEY NICKEL, AND SIMULATION OF'CHAIN GROWTH IN THE FISCHER-TROPSCH SYNTHESIS
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1 .. '.... ~mthanation OF CARBON MONOX~DE AND CARBON DIOXIDE ON RANEY NICKEL, AND COMPUTE~ SIMULATION OF'CHAIN GROWTH IN THE FISCHER-TROPSCH SYNTHESIS.,. j I l! 1!,i By, (5) CHUNG BOON LEE, B. ENG... \ I 1,, A Thesis Submitted to the Faculty of Graduate Studies in'partial F~lfilment of the Requirements... "."... for the Degree Doctor of Philosophy.. / ~.,-, McMaster University November, r- ~---,,=7":'" ~ :'.I.,;:-.l' ~"
2 i (,. 'i I j..', METHANATION OF CARBON OXIDES \ '.. ON RANEY NICKEL AND SIMULATION OF CHAIN GROWTH IN FISCHER-TROPSCH SYNTHESIS.. --',. f.; '. " ".. L
3 ;.. or,, DOCTOR bf PHILOSOPHY (1982) (Chemical Engi~eering) TITLE: ~c- I McMASTER UNIVE~SITY. Hamilton, Ontario. ~ation of Carbon Monoxide and Carbon Dioxide on Raney' Nickel, and Computer Simulation of Chain Growth in the fischer-tropsch Synthesis, AUTl{OR: SUPERVISOR: Chung Boon Lee, B. Eng. (McMaster University) Professor R. B. Anderson i j NUMBE~ OF PAGES: 381, xv :....."..... ~ ii }.... ~
4 " /... j! To Marilyn '".,. ',;. "1. I I \ I I I II! ", and To my P,a,rertts, /, I Ii I -' '. ' " I,.,,.., '. 0. " I " L I _""_n. _-,---;'_'_--.,---.- J
5 r.' L.,.. ABSTRACT The methanation of carbon monoxide and carbon dioxide was studied over Raney nickel. characterize4 by chemisorption techniques. The catalyst was,. A differential p.~rg-fi6w reactor was used to obtain kinetic data. The to. ~ \ J~.~. reactio~ rates were in~stigated as a function of temperature, reactants and products concentrations. was foun~~equat~ in, representin~ the k~netic The power rate law data of carbon d~oxide methanation. The orders of reaction for hydro- I ' gen and carbon monoxide were' ob~ained. Carbonaceous species were found on the catalyst surface after methanation reaction, which could react with hydrogen to give methane. MUltilayers of,carbon 'pec~es were depo~ited on~e, catalyst surface dur- ing CO methanation; less than ~ monolayer was found when carbon dioxide was used as feed. The effects of reaction conditions on the amount of residual carbon was -- also investigated.. The data in general agre~1 wit~ a mechanism involving } the hydrogenation of carbonaceous species as the rate determining step. The differences between CO and CO 2 methanations were ".also discussed. The carbon chain growth process in the Fischer-~ropsch \ synthesis was simulated using available data in the literature iii l,..,,, -.',.._,
6 .I The simulation was done by representing the hyd rocar~on chains by numbers stored in vectorj. Variou3 chain growth schemes were tested. process..could The results ~ involve the suggested that t~e step~ise additions carbon chain growth of both one7carbon and two-carbon. units : (..,"'.,... I.. iv ; L
7 " ACKNOWLEDGEMENTS."t. ~ lo ~". 1:'". ~. -'. '.."," The ~uthor wishes to acknowledge his appreciation to those people who.have contributed to this wo~k. The author is indebted to his research direotor,,. Professor. R.B. Anderson, for his guidance, support and patience. Th~, -.r.-.. ".'...,..~, contributions of Dr. ~.H.I..ird,, " Dr. J. Vlachopoulos and Dr. W.W. Smeltzer, members of the supervisory committee, are,also acknowledged. Special thanks a~e her encouragement and patience. due to his wife, Marilyn for Financia~ ~ssistance provided by the D~partment of Chemical Engineering and the National Research COUncil of Canada was also gratefully accepted. i! i I I I,.1,.... ".--,v L,.'
8 TABLE OF CONTENTS PAGE Chapter 1 Introduction 1 1.'1 General Methanation of Carbon Monoxide Mechanism of Carbon Monoxide Methanation ~ Xinetic Studies Infrared Spectra Studies P~soning and Other Studies 26 Chapter 2 Chapter Methan~tion of Carbon Dioxide 1.4 Thermodynamics of Methanation 1.5 Reactor 1.6 Analysis of Data 2.1 Characterization of Catalyst i":~';~',:,.. ~... 'Ci '..rodilction 2.2 Adsorption Studies 2 '-2: 1 General 2,2.2 Nitrogen Adsorption Pore Size Distribution Chemisorption Experimental 3.1 Materials O 3.2 Flow System 28 ' o! L. vi
9 3.3 The Reactor 3.4 Operating Procedure Interparticle Mass and Heat Transfer Intraparticle Mass and Heat Transfer 86. Chapter 4 Carbon Monoxide Methanation Introduction Preliminary Kinetic~Studies Kinetics Effect of Temperature Effects of Reactants and Products Reduction of Carbonaceous Residues Mechknistic Considerations 134 Chapter 5 Carbon Dioxide Methanat Introduction Preliminary Kinetic :3 Kinetics Effect of Effects of Reactants and Products Reduction of Carbonaceous Residues Mechanistic Considerations 203.,. Chapter 6 Chain Growth in the Fischer-Tropsch Synthesis Introduction Literature Survey 220 vii _._.-,',...:.-... :... ~. \
10 '. PAGE 6.3 Formalism of ~hain Growth Schemes Computer Simulation of Chain Growth Estimation of Growth Constants Organization of Programs 250 &.7 Results and Discussion 252 Chapter General Chain Growth Carbon Number Distribution Conclusions I I!.1 I i I. I. Appendix A Appendix B Appendix C References Analysis by Gas Chromatography Calculation Procedures B.l Calculation of Conversion and Rate of Reaction B.2 Parameter Estimation Derivation of Rate Equations ,,!.., Appendix. D Tables of Experimental Data' 324 viii,.l _-_._~----- '"
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