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Catalyctic Reduction of Nitric Oxide by Carbon Monoxide and Copper Loaded Granular Activated Carbon in the Presence of Oxygen

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Catalyctic Reduction of Nitric Oxide by Carbon Monoxide and Copper Loaded Granular Activated Carbon in the Presence of Oxygen New Jersey Institute of Technology Digital Commons @ NJIT Theses Electronic Theses and Dissertations Spring 5-31-1998 Catalyctic reduction of nitric oxide by carbon monoxide and copper loaded granular activated carbon in the presence of oxygen Kaiwen Ma New Jersey Institute of Technology Follow this and additional works at: https://digitalcommons.njit.edu/theses Part of the Chemistry Commons Recommended Citation Ma, Kaiwen, "Catalyctic reduction of nitric oxide by carbon monoxide and copper loaded granular activated carbon in the presence of oxygen" (1998). Theses. 940. https://digitalcommons.njit.edu/theses/940 This Thesis is brought to you for free and open access by the Electronic Theses and Dissertations at Digital Commons @ NJIT. It has been accepted for inclusion in Theses by an authorized administrator of Digital Commons @ NJIT. For more information, please contact [email protected]. Copyright Warning & Restrictions The copyright law of the United States (Title 17, United States Code) governs the making of photocopies or other reproductions of copyrighted material. Under certain conditions specified in the law, libraries and archives are authorized to furnish a photocopy or other reproduction. One of these specified conditions is that the photocopy or reproduction is not to be “used for any purpose other than private study, scholarship, or research.” If a, user makes a request for, or later uses, a photocopy or reproduction for purposes in excess of “fair use” that user may be liable for copyright infringement, This institution reserves the right to refuse to accept a copying order if, in its judgment, fulfillment of the order would involve violation of copyright law. Please Note: The author retains the copyright while the New Jersey Institute of Technology reserves the right to distribute this thesis or dissertation Printing note: If you do not wish to print this page, then select “Pages from: first page # to: last page #” on the print dialog screen The Van Houten library has removed some of the personal information and all signatures from the approval page and biographical sketches of theses and dissertations in order to protect the identity of NJIT graduates and faculty. ABSTRACT CATALYTIC REDUCTION OF NITRIC OXIDE BY CARBON MONOXIDE AND COPPER LOADED GRANULAR ACTIVATED CARBON IN THE PRESENCE OF OXYGEN by Kaiwen Ma The reduction reaction of nitric oxide (NO) by carbon monoxide (CO), and granular activated carbon (GAC) in the presence and absence of oxygen was studied in a fixed bed catalytic reactor. The conversion of NO as a function of reaction temperature was evaluated for various reductant to NO ratios and space velocities. The results show that oxygen enhanced the NO+CO reaction over copper (Cu) ion exchanged ZSM-5. About 60% NO conversion to nitrogen (N2) was obtained at 400°C and 2,000 v/v/hr. This result is consistent with the hypothesis that CO is an intermediate in the soot-NO reaction. The apparent mechanism seems to be the soot-02 reaction produces CO on the surface, the CO diffuses into the catalyst pores where it preferentially reacts with NO to produce carbon dioxide (CO-) and N2. The overall observation is that soot or GAC in the presence of oxygen reduces NO to N2 and CO2 if a Cu containing catalyst is present. One observes that Cu ion dispersed in GAC in the presence of 10% oxygen promotes the formation of CO at a relatively low temperature. This is followed by essentially complete NO conversion to N2 at 600°C and 2,000 v/v/hr and 20,000 v/v/hr. At 450°C, 95% NO is converted to N2 at 2,000 v/v/hr. The reaction rate of NO conversion to N2 decreases with increasing space velocity with either CO or carbon black as the reducing materials. Based on the results presented here, additional research on the catalytic reduction of NO by CO on the results presented here, additional research on the catalytic reduction of NO by CO and copper loaded GAC in the presence of 0, at higher space velocities between 50,000 and 100,000 v/v/hr is warranted. Effect of water on the two reactions is also needed to be studied. CATALYTIC REDUCTION OF NITRIC OXIDE BY CARBON MONOXIDE AND COPPER LOADED GRANULAR ACTIVATED CARBON IN THE PRESENCE OF OXYGEN by Kaiwen Ma A Thesis Submitted to the Faculty of New Jersey Institute of Technology in Partial Fulfillment of the Requirements for the Degree of Master of Science in Applied Chemistry Department of Chemical Engineering, Chemistry, and Environmental Science May 1998 APPROVAL PAGE CATALYTIC REDUCTION OF NITRIC OXIDE BY CARBON MONOXIDE AND COPPER LOADED GRANULAR ACTIVATED CARBON IN THEPRESENCE OF OXYGEN Kaiwen Ma Dr. Henry Shaw, Thesis Advisor Date Professor of Chemical Engineering, Chemistry, and Environmental Science, NJIT b Dr. Robert Pfeffer, Thesis Advisor Date Professor of Chemical Engineering, Chemistry, and Environmental Science, NJIT Dr. JamesGr ow, Committee Member Date Associat Professor of Chemical Engineering, Chemistry, and Environmental Science, NJIT BIOGRAPHICAL SKETCH Author: Kaiwen Ma Degree: Master of Science in Applied Chemistry Date: May 1998 Undergraduate and Graduate Education: • Master of Science in Applied Chemistry, New Jersey Institute of Technology, Newark, New Jersey, 1998 ® Bachelor of Science in Applied Chemistry, New Jersey Institute of Technology, Newark, New Jersey, 1996 Major: Applied Chemistry This thesis is dedicated to my beloved parents and my fiancee ACKNOWLEDGEMENT I would like to express my deepest appreciation to Dr. Henry Shaw and Dr. Robert Pfeffer, who not only served as my research advisors, providing valuable and countless resources, insight, and intuition, but also gave me support, encouragement, and reassurance. Special thanks are given to Dr. James Grow for actively participating in my committee. Many of my fellow graduates in the ATC building are deserving of recognition for their support. I also wish to thank Dr. Istvan Bágyi for his assistance in the past year. vi TABLE OF CONTENTS Chapters Page 1 INTRODUCTION 1 2 EXPERIMENTAL 11 2.1 Experimental Apparatus 11 2.2 Instruments and Chemicals 11 2.2.1 Reactor 11 2.2.2 Gas Chromatography 13 2.2.3 Thermgravimetric(TGA) 14 2.2.4 X-ray Diffraction 15 2.2.5 Chemicals 16 2.3 Experimental Procedure 17 2.3.1 Fixed Bed Gas Experimental Procedure 17 2.3.2 Preparation of CuO on Carbon Black and Gamma Alumina 18 3 RESULTS AND DISCUSSION 20 3.1 Reduction of NO by CO over Cu-ZSM-5 70 3.1.1 Effect of Oxygen Concentration 22 3.1.2 Effect of CO Concentration 23 3.1.3 Effect of Space Velocity 23 3.2 Reduction of NO by Granular Activated Carbon (GAC) 25 3.2.1 Reduction of NO by GAC with 10% Oxygen Cu-ZSM-5 25 vii TABLE OF CONTENTS (Continued) Chapters Page 3.2.1.1 Effect of Space Velocity 25 3.2.2 Reduction of NO by Cu ion /GAC with 10% Oxygen 27 3.2.2.1 Effect of Space Velocity on GAC Reduction with 20% Cu ion 29 3.2.3 Reduction of NO by GAC with 10% Oxygen 32 3.2.3.1 Effect of Space Velocity 32 3.3 Effect of Copper Ion on NO Reduction by Propane with 10% Oxygen over γ-Al2O3 32 3.4 Thermogravimetric Analysis 33 3.5 X-ray Diffraction Crystallography 33 4 CONCLUSIONS 35 APPENDIX A FIGURES OF EXPERIMENT RESULTS 37 REFERENCES 54 viii LIST OF TABLES Tables Page 2.1 Operations Conditions of HP 5860A 14 2.2 The Parameters Used in TGA Analysis 15 ix LIST OF FIGURES Figures Page 2.1 Schematic Diagram of Experimental Apparatus 12 3.1 Effingham Diagram 38 3.2 Reduction of NO by CO in the Presence and Absence of Oxygen; GHSV = 2,000,[NO]i = [CO]i = 500 ppm 39 3.3 CO2 Produced in the Reduction of NO by CO in the Absence of Oxygen, GHSV = 2,000, over Cu-ZSM-5 40 3.4 Oxidation of CO by O2 over Cu-ZSM-5; GHSV = 2,000 41 3.5 Effect of Oxygen Concentration on NO Reduction by CO over Cu-ZSM-5 at 400°C; [NO]i = [CO]i= 490 ppm, GHSV = 2,000 42 3.6 Effect of CO to NO Concentration Ratio on NO Reduction over Cu-ZSM-5; GHSV = 2,000, 10% Oxygen 43 3.7 Effect of Oxygen Concentration on NO Reduction by CO over Cu-ZSM-5; GHSV = 2,000, [CO]; = 2[NO]i 44 3.8 Effect of Space Velocity on NO Reduction by CO over Cu-ZSM-5; [NO]i = [CO]i = 490 ppm, 10% Oxygen 45 3.9 Effect of [CO]/[NO] Mole Ratio on NO Reduction by CO over Cu-ZSM-5; GHSV = 20,000, 10% Oxygen 46 3.10 Effect of Space Velocity on Reduction of NO by Activated Carbon Presented as 5% GAC over 95% Cu-ZSM-5; [NO]; = 590 ppm, 10% Oxygen 47 3.11 Effect of Space Velocity on the Reduction of NO by 20% Copper Loaded GAC; [NO]i = 590 ppm, 10% Oxygen 48 3.12 Reaction of GAC with 10% Oxygen over Different Catalysts 49 3.13 Effect of Space Velocity on Reduction of NO by GAC; [NO] = 590 ppm, 10% Oxygen 50 LIST OF FIGURES (Continued) Figures Page 3.14 Effect of Cu Ion on the Reduction of NO by C3H8 over Gamma-Alumina; [NO]i = 400 ppm, [C3H8]i = 500 ppm, 10% Oxygen, GHSV = 2,000 51 3.15 TGA for Decomposition of Cu(NO3)2.3H2O to CuO 52 3.16 X-ray Diffraction Pattern of 20% Copper Loaded Alumina 53 xi CHAPTER 1 INTRODUCTION Air pollution from mobile sources is an increasingly serious problem throughout most of the industrialised world.
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