Direct Low Temperature Oxidation of Methane to Methanol Via Copper Zeolite Materials PDF Download
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Author: Barbra Eva Schaller
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Author: Barbra Eva Schaller
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Author: Karthik Narsimhan
Publisher:
ISBN:
Category :
Languages : en
Pages : 147
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Book Description
As production of shale gas has increased greatly in the United States, the amount of stranded shale gas that is flared as carbon dioxide has become significant enough to be considered an environmental hazard and a wasted resource. The conversion of methane, the primary component of natural gas, into methanol, an easily stored liquid, is of practical interest. However, shale wells are generally inaccessible to reforming facilities, and construction of on-site, conventional methanol synthesis plants is cost prohibitive. Capital costs could be reduced by the direct conversion of methane into methanol at low temperature. Existing strategies for the partial oxidation of methane require harsh solvents, need exotic oxidizing agents, or deactivate easily. Copper-exchanged zeolites have emerged as candidates for methanol production due to high methanol selectivity (> 99%), utilization of oxygen, and low reaction temperature (423-473 K). Despite these advantages, three significant shortcomings exist: 1) the location of surface intermediates on the zeolite is not well understood; 2) methane oxidation is stoichiometric, not catalytic; 3) there are few active sites and methanol yield is low. This work addresses all three shortcomings. First, a new reaction pathway is identified for methane oxidation in copper-exchanged mordenite zeolites using tandem methane oxidation and Koch carbonylation reactions. Methoxy species migrate away from the copper active sites and adsorb onto Bronsted acid sites, signifying spillover on the zeolite surface. Second, a process is developed as the first instance of the catalytic oxidation of methane into methanol at low temperature, in the vapor phase, and using oxygen as the oxidant. A variety of commercially available copper-exchanged zeolites are shown to exhibit stable methanol production with high methanol selectivity. Third, catalytic methanol production rates and methane conversion are further improved 100- fold through the synthetic control of copper speciation in chabazite zeolites. Isolated monocopper species, directed through the one-pot synthesis of copper-exchanged chabazite zeolites, correlates with methane oxidation activity and is likely the precursor to the catalytic site. Together, these synthetic methods provide guidelines for catalyst design and further improvements in catalytic activity.
Author: D.M. Bibby
Publisher: Elsevier
ISBN: 0080960707
Category : Technology & Engineering
Languages : en
Pages : 759
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Book Description
This proceedings volume comprises the invited plenary lectures, contributed and poster papers presented at a symposium organised to mark the successful inauguration of the world's first commercial plant for production of gasoline from natural gas, based on the Mobil methanol-to-gasoline process. The objectives of the Symposium were to present both fundamental research and engineering aspects of the development and commercialization of gas-to-gasoline processes. These include steam reforming, methanol synthesis and methanol-to-gasoline. Possible alternative processes e.g. MOGD, Fischer-Tropsch synthesis of hydrocarbons, and the direct conversion of methane to higher hydrocarbons were also considered.The papers in this volume provide a valuable and extremely wide-ranging overview of current research into the various options for natural gas conversion, giving a detailed description of the gas-to-gasoline process and plant. Together, they represent a unique combination of fundamental surface chemistry catalyst characterization, reaction chemistry and engineering scale-up and commercialization.
Author: Vladimir Arutyunov
Publisher: Elsevier
ISBN: 0444632514
Category : Technology & Engineering
Languages : en
Pages : 321
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Book Description
Direct Methane to Methanol: Foundations and Prospects of the Process offers a state-of-the-art account of one of the most interesting and potentially commercial technologies for direct conversion of natural gas into valuable chemicals. The book thoroughly explains the complex and unusual chemistry of the process, as well as possible applications for direct methane to methanol (DMTM). It covers topics involving thermokinetics, pressure, direct oxidation of heavier alkanes, and more, and provides detailed appendices with experimental data and product yields. This book provides all those who work in the field of gas processing and gas chemistry with the theory and experimental data to develop and apply new processes based on direct oxidation of natural gas. All those who deal with oil and natural gas production and processing will learn about this promising technology for the conversion of gas into more valuable chemicals. - Reviews more than 350 publications on high-pressure, low-temperature oxidation of methane and other gas phase hydrocarbons - Contains rare material available for the first time in English - Explains the reasons of previous failure and outlines the way forward for commercial development of the conversion technology - Presents a deep theoretical knowledge of this complex conversion process
Author: Annemie Bogaerts
Publisher: MDPI
ISBN: 3038977500
Category : Technology & Engineering
Languages : en
Pages : 248
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Book Description
Plasma catalysis is gaining increasing interest for various gas conversion applications, such as CO2 conversion into value-added chemicals and fuels, N2 fixation for the synthesis of NH3 or NOx, methane conversion into higher hydrocarbons or oxygenates. It is also widely used for air pollution control (e.g., VOC remediation). Plasma catalysis allows thermodynamically difficult reactions to proceed at ambient pressure and temperature, due to activation of the gas molecules by energetic electrons created in the plasma. However, plasma is very reactive but not selective, and thus a catalyst is needed to improve the selectivity. In spite of the growing interest in plasma catalysis, the underlying mechanisms of the (possible) synergy between plasma and catalyst are not yet fully understood. Indeed, plasma catalysis is quite complicated, as the plasma will affect the catalyst and vice versa. Moreover, due to the reactive plasma environment, the most suitable catalysts will probably be different from thermal catalysts. More research is needed to better understand the plasma–catalyst interactions, in order to further improve the applications.
Author: National Academies of Sciences, Engineering, and Medicine
Publisher: National Academies Press
ISBN: 0309483360
Category : Science
Languages : en
Pages : 257
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Book Description
In the quest to mitigate the buildup of greenhouse gases in Earth's atmosphere, researchers and policymakers have increasingly turned their attention to techniques for capturing greenhouse gases such as carbon dioxide and methane, either from the locations where they are emitted or directly from the atmosphere. Once captured, these gases can be stored or put to use. While both carbon storage and carbon utilization have costs, utilization offers the opportunity to recover some of the cost and even generate economic value. While current carbon utilization projects operate at a relatively small scale, some estimates suggest the market for waste carbon-derived products could grow to hundreds of billions of dollars within a few decades, utilizing several thousand teragrams of waste carbon gases per year. Gaseous Carbon Waste Streams Utilization: Status and Research Needs assesses research and development needs relevant to understanding and improving the commercial viability of waste carbon utilization technologies and defines a research agenda to address key challenges. The report is intended to help inform decision making surrounding the development and deployment of waste carbon utilization technologies under a variety of circumstances, whether motivated by a goal to improve processes for making carbon-based products, to generate revenue, or to achieve environmental goals.
Author: Yong-jun Gao
Publisher: Springer Nature
ISBN: 303074406X
Category : Technology & Engineering
Languages : en
Pages : 871
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Book Description
This books provides a comprehensive platform to the scientific, education and research communities working on various fields related to sustainable energy. It covers the exploration, generation and application of this area to meet societal needs as well as addressing global issues related to the environment. The content of this book presents research related to energy and how to tackle climate change as a comprehensive framework based on the success of the Millennium Development Goals (MDGs). The authors use the scientific method to analyze and deliver viable technical solutions, demonstrating how chemistry and engineering can be combined to solve technically challenging problems. While maintaining high scientific rigor, a quantitative approach is offered in select chapters to the study of energy related to our societies increasing need for electrical and chemical energy feedstocks.
Author: I. Chorkendorff
Publisher: John Wiley & Sons
ISBN: 3527605649
Category : Science
Languages : en
Pages : 469
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Book Description
Until now, the literature has offered a rather limited approach to the use of fundamental kinetics and their application to catalytic reactions. Subsequently, this book spans the full range from fundamentals of kinetics and heterogeneous catalysis via modern experimental and theoretical results of model studies to their equivalent large-scale industrial production processes. The result is key knowledge for students at technical universities and professionals already working in industry. '... such an enterprise will be of great value to the community, to professionals as well as graduate and undergraduate students attempting to move into the field of modern catalysis and kinetics. I strongly recommend you publish this book based on the proposal.' - Prof. Dr. G. A. Samorjai, University of California 'Both authors are well respected specialists, with a very long record of original top-quality work and an international reputation. A book from these authors will be considered an authoritative piece of work, I definitely support this project and I am looking forward to use the book when published.' - Prof. Dr. D. E. Resasco, University of Oklahoma 'I wholly support the proposed project. The authors are very competent young colleagues and there is a real need for such a textbook' - Prof. Dr. G. Ertl, Fritz-Haber-Institut, Max-Planck-Gesellschaft, Berlin
Author: Allegra Latimer
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Generally, this failure has been attributed to two primary difficulties: (1) the high barriers required to activate methane (activity), and (2) the higher activity of the C-H bonds in methanol compared to methane (selectivity). In this thesis, we delve into both of these problems and identify general frameworks and strategies that can be used in future research to identify promising catalyst materials. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. We combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates, and successfully rationalize the available empirical data across catalyst classes. We then extend this analysis to catalysts that proceeed via a surface-stabilized transition state for methane activation. We present a framework for predicting the transition state's geometry (radical or surface-stabilized) and its approximate energy on a given active site. We then shift our attention to understanding and optimizing selectivity. First, we determine the principles guiding the selectivity of a related reaction, direct methanol to formaldehyde on ruthenium oxide catalysts, and find that limiting electrophilic surface oxygen coverage for this reaction is key to obtaining high selectivity. Next, recognizing that a precise and general quantification of the limitations of catalytic direct methane to methanol has not yet been established, we present a simple kinetic model to explain the selectivity-conversion tradeoff that hampers continuous partial oxidation of methane to methanol. Stemming from this analysis, we suggest several design strategies for increasing methanol yields under the constraint of the selectivity-conversion tradeoff. These strategies include (1) "collectors, " materials with strong methanol adsorption potential that can help to lower the partial pressure of methanol in the gas phase, (2) aqueous reaction conditions, and/or (3) diffusion-limited systems. Having identified these strategies, we work towards realizing a system capitalizing on (2), aqueous reaction conditions, by collaborating with experimental colleagues to develop a low-temperature electrochemical approach for methane oxidation. It is the general aim of this thesis to develop straightforward, accessible models with the help of Density Functional Theory that yield generalizable insights. We are hopeful that the models presented herein may provide a reliable framework for future researchers working to understand and evaluate new catalysts and processes for the direct oxidation of methane to methanol.
Author: Martin Bertau
Publisher: Springer Science & Business Media
ISBN: 3642397093
Category : Technology & Engineering
Languages : en
Pages : 699
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Book Description
Methanol - The Chemical and Energy Feedstock of the Future offers a visionary yet unbiased view of methanol technology. Based on the groundbreaking 1986 publication "Methanol" by Friedrich Asinger, this book includes contributions by more than 40 experts from industry and academia. The authors and editors provide a comprehensive exposition of methanol chemistry and technology which is useful for a wide variety of scientists working in chemistry and energy related industries as well as academic researchers and even decision-makers and organisations concerned with the future of chemical and energy feedstocks.
