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Role of Benzene, Toluene and Xylene to Acid Gas Destruction

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Role of Benzene, Toluene and Xylene to Acid Gas Destruction ABSTRACT Title of Document: ROLE OF BENZENE, TOLUENE AND XYLENE TO ACID GAS DESTRUCTION IN THERMAL STAGE OF CLAUS REACTORS Salisu Ibrahim, Ph.D. Directed By: Ashwani K. Gupta, Distinguished University Professor, Department of mechanical Engineering Crude oil and natural gas often contain acid gases (H2S and CO2) and trace amounts of benzene, toluene and xylene (BTX) and these are all harmful to human health, environment and industrial equipment. Acid gases in chemical industry and vehicles cause corrosion to parts of engines, refinery equipment and catalysts deactivation in catalytic processes. Human exposure to H2S, even in low concentrations, causes burning of eyes, headache, dizziness, dyspnea, and skin irritations. Inhalation of high doses of BTX may cause skin and respiratory tract irritation. Increased energy demand and exploitation of sourer feedstock have made regulatory agencies worldwide to promulgate stricter regulations on sulfur emissions. US EPA requires a reduction of sulfur in gasoline from 30ppm to 10ppm by 2017. Crude oil and gas must be subjected to more efficient desulfurization processes. The separated acid gases and BTX is further processed in Claus process for chemical and energy recovery. Currently, BTX poses several technical and operational problems that result in higher operational costs and increased toxic gas emissions in Claus plants. BTX destruction in the thermal stage of Claus process was identified as the solution. Acid gas and BTX combustion in thermal stage of Claus reactor, which provides simultaneous recovery of both sulfur and thermal energy, is the subject of this research. Effect of BTX in H2S fueled flames on sulfur chemistry in thermal stage of a Claus reactor was characterized. Reactor conditions that promote BTX destruction are presented. Oxygen enriched combustion air for the destruction of BTX and acid gas is examined. Chemical kinetic pathways of BTX destruction under high temperature conditions of the Claus reactor are evaluated. Intermediate radicals and stable species formed during the combustion process are characterized using flame emission spectroscopy and gas chromatography (GC). Role of multiple contaminants, CO2 and benzene, toluene or xylene in H2S combustion is also investigated. Chemical kinetic pathways and reactor conditions that promote/hinder the formation of mercaptans (such as COS and CS2) is addressed. The results presented here assist in the design guidelines of advanced Claus reactors for enhanced sulfur capture in the thermal stage and to mitigate environmental issues. ROLE OF BENZENE, TOLUENE AND XYLENE TO ACID GAS DESTRUCTION IN THERMAL STAGE OF CLAUS REACTORS By Salisu Ibrahim Dissertation submitted to the Faculty of the Graduate School of the University of Maryland, College Park, in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy 2015 Advisory Committee: Professor Ashwani K. Gupta, Chair Professor Jungho Kim Associate Professor Nam S. Wang, Dean’s Representative Associate Professor Bao Yang Associate Professor Ahmed S. Al Shoaibi © Copyright by Salisu Ibrahim 2015 Dedication This dissertation is dedicated to Almighty Allah for giving me the strength to complete this work, my parents (Ahmadu Ibrahim Guja and Mairo Ibrahim) for their mental support, my mentors for believing in my abilities, and all well-wishers. ii Acknowledgments This dissertation represents the result of my fruitful experience at the Combustion Engineering laboratory, University of Maryland College Park. I am sincerely grateful to Professor Ashwani K. Gupta for offering me the opportunity to work in Combustion Engineering laboratory. Professor Gupta’s consistent demand for hard-work and productivity shaped my research aptitude and confidence that resulted in the timely completion of this dissertation. I am also very grateful to Associate Professor Ahmed S. Al Shoaibi of the Petroleum Institute Abu Dhabi who encouraged and supported me to join the PhD program at University of Maryland. Associate Professor Al Shoaibi has continued to inspire and support me throughout the course of my PhD program. He offered valuable contributions and supported in sourcing the finances used for this research investigation. My sincere appreciation also goes to members of my dissertation committee, Professor Jungho Kim, Associate Professor Nam S. Wang and Associate Professor Bao Yang for their efforts, advice and support. I would like to extend my gratitude to the current and former team members of the Combustion Engineering laboratory. They offered me great support and valuable input, especially in setting up my experiments. The enormous gratitude to my parents cannot be expressed in words. It has been over a decade since I left them in pursuit of my academic and career development. I sincerely appreciate their relentless support and patience while away from them. Also, I would like to thank my fiancée, Zainab A. Auwal for her support and understanding during the most stressful iii part of my PhD program. I would like to extend my gratitude to my friends for their support and encouragements. Finally, I acknowledge the research and financial support provided by The Petroleum Institute, Abu Dhabi, ADNOC and GASCO. iv v Table of Contents Dedication… ................................................................................................................. ii Acknowledgments........................................................................................................ iii Table of Contents ......................................................................................................... vi List of Tables ............................................................................................................... xi List of Figures ............................................................................................................. xii Numenclature ............................................................................................................ xxii Chapter 1 Introduction ............................................................................................... 1 1.1 Environmental and Health Challenges of Acid Gas .......................................... 1 1.2 Regulation on Sulfur Content in Fuels ............................................................... 3 1.3 Separation of Acid Gas from Crude oil and Gas................................................ 4 1.3.1 Hydro-Desulfurization ..................................................................... 4 1.3.2 Oxidative Desulfurization ................................................................ 5 1.3.3 Bio-Catalytic Desulfurization .......................................................... 7 1.3.4 Adsorptive Desulfurization (ADS) .................................................. 7 1.3.5 Amine Extraction ............................................................................. 8 1.4 Treatment of Acid Gas ....................................................................................... 9 4.4.1 Claus Thermal Stage ...................................................................... 11 1.4.2 Claus Catalytic Stage ..................................................................... 12 1.5 Research Motivations ....................................................................................... 14 1.6 Research Objectives ......................................................................................... 15 Chapter 2 Literature Review.................................................................................... 17 vi 2.1 Reaction Mechanisms of H2S Combustion ...................................................... 17 2.2 Experimental Characterization of H2S Combustion ........................................ 20 2.3 Practical Challenges of Sulfur Recovery ......................................................... 26 2.4 Challenges of COS and CS2 in Sulfur Recovery ............................................. 30 2.5 Sulfur Recovery via H2S Pyrolysis .................................................................. 33 2.6 BTX Thermal Decomposition .......................................................................... 36 2.6.1 Xylene Thermal Decomposition .................................................... 38 2.6.2 Toluene Thermal Decomposition .................................................. 43 2.6.3 Benzene Thermal Decomposition .................................................. 57 Chapter 3 Experimental Facility .............................................................................. 65 3.1 Experimental Setup .......................................................................................... 65 3.2 Flow Meters. .................................................................................................... 67 3.3 Gas Sampling Probe ......................................................................................... 67 3.4 Diagnostics and Safety Gas Detectors ............................................................. 68 3.5 Systematic Error ............................................................................................... 69 Chapter 4 Results and Discussion ........................................................................... 71 4.1 Benzene, Toluene or Xylene Addition Effects to H2S Combustion ................ 71 4.1.1 Toluene Addition Effects to H2S/O2 Flame ................................... 72 4.1.1.1 Analysis of Combustion Products ............................................... 73 4.1.1.2 Summary
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