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Return to DOE Reports Table of Contents A-H Iron-Induced Deactivation of Supported Nickel Methanation Catalysts - 1978. Dumesic, James A. University of Wisconsin In this pdf format, this document has 161 pages and is 4.61 MB. Table of Contents I. Mossbauer Spectroscopy Cell for in situ Catalyst Characterization and Reaction Kinetics studies at high pressure 7 I. A. Introduction 7 I. B. Apparatus 4 I.B.1. The High-Pressure Cell 9 I.B.2. The Prereactor and Postreactor 12 I.C. Performance 12 I.D. References 19 II. Deactivation Studies of Ni/Al2O3 Methanation Catalysts 28 II.A. Experimental 29 II.B. Results 31 II.C. Discussion 33 II.D. Conclusions 40 II.E. References 42 III. Appendix A. Criteria for Stable Ni Particle size under Methanation Reaction Conditions: Nickel Transport and Particle Size Growth via Nickel Carbonyl 62 III.A. Experimental 63 III.A.1. High Pressure Reaction System 63 III.A.2. Particle Size Determinations 64 III.A.3. Catalyst reparation and Treatment 64 III.B. Results 67 III.C. Discussion 70 III.C.1. Nickel Transportation and Particle Size Growth 70 III.C.2. Kinetic and Thermodynamic Aspects of Ni(CO)4 Formation 74 III.C.3. Blockage of Surface Sites 79 III.C.4. Methanation Kinetics 80 III.D. Conclusions 82 III.E. References 83 IV. Appendix B - Iron Pentacarbonyl Decomposition over Grafoil 97 IV. Production of Small Metallic Iron Particles 97 IV.A. Experimental 98 IV.A.1. Iron Pentacarbonyl Handling 98 IV.A.2. Mossbauer Spectroscopy 99 IV.A.3. Graphite Sample 100 IV.B. Results 100 IV.C. Discussion 102 IV.C.1. Fe(CO)5 Adsorbed on Graphite – Spectrum 1 102 IV.C.2. Interaction of Metallic Iron with Graphite Spectra 2, 3, and 4 103 IV.C.3. Quantitative Spectral Analysis – Spectra 2 and 3 107 IV.C.4. Proposed Iron Morphology 113 IV.D. 115 V. Appendix C. Iron Pentacarbonyl Decomposition over Grafoil 133 V. Effect of Sample Outgassing on Decomposition Kinetics 133 V.A. Experimental 134 V.A.1. Graphite Sample 134 V.A.2. Mossbauer Spectroscopy 134 V.A.3. Volumetric Gas Phase Measurements 135 V.B. Results 137 V.B.1. Mossbauer Spectroscopy 137 V.B.2. Volumetric Gas Phase Measurements 138 V.C. Discussion 140 V.C.1. Mossbauer Spectroscopy 140 V.C.2 Volumetric Gas Phase Measurements 142 V.D. Conclusions 148 V.E. References 149 | |||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||