Novel Catalytic Materials for Carbon Dioxide Reforming of Methane Under Severly Deactivating Conditions PDF Download
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Author: Susan Michelle Stagg-Williams
Publisher:
ISBN:
Category : Carbon dioxide
Languages : en
Pages : 364
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Author: Susan Michelle Stagg-Williams
Publisher:
ISBN:
Category : Carbon dioxide
Languages : en
Pages : 364
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Author: Jain-Kai Hung
Publisher:
ISBN:
Category : Catalysts
Languages : en
Pages : 438
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Author: Xian Cao
Publisher:
ISBN:
Category : Carbon dioxide
Languages : en
Pages : 150
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Author:
Publisher:
ISBN:
Category : Dissertations, Academic
Languages : en
Pages : 708
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Author: Bahman Zohour
Publisher:
ISBN:
Category :
Languages : en
Pages : 168
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The goal of this research is to explore novel catalytic material and systems for effective conversion of C1 feed. Catalysis of C1 chemistry is of critical importance for the clean production of fuels and chemicals and future energy sustainability. Herein, two processes were studied: In the first section, a comprehensive study of oxidative coupling of methane (OCM) using novel nanofiber catalysts of mixed metal oxides was undertaken and in the second section, direct catalytic conversion of carbon dioxide (CO2) to methanol was studied, which resulted in discovery of a superior catalytic system for CO2 hydrogenation to methanol. Section 1: Utilization of natural gas as an alternate chemical feedstock to petroleum has been a highly desirable but difficult goal in industrial catalysis. Accordingly, there has been a substantial interest in the oxidative coupling of methane (OCM), which allows for the direct catalytic conversion of methane into economically valuable C2+ hydrocarbons. OCM is a complex reaction process involving heterogeneous catalysis intricately coupled with gas phase reactions; hence, despite decades' worth of research, it has yet to be commercialized. The lack of progress in OCM is primarily due to the following reasons: 1. The absence of a highly active and robust catalyst that can operate at lower temperatures; and 2. Our inadequate understanding of the underlying detailed chemical kinetics mechanism (DCKM) of the OCM process, which impedes the undertaking of quantitative simulations of novel reactor configurations and/or operating strategies. To address these issues, we undertook the following program of studies: 1. Further improved the synthesis of novel nanofiber catalysts by electrospinning, building on the early discovery that La2O3-CeO2 nanofibers were highly active and robust OCM catalysts; 2. Applied our novel microprobe sampling system to OCM reactors for the acquisition of spatially resolved species concentration and temperatures profiles within the catalytic zone. Our novel sampling approach led to the important discovery that H2 is produced very early in the OCM catalytic zone, an observation that was completely missed in all prior studies. The application of our novel microprobe system to a dual-bed OCM reactor also demonstrated the feasibility to significantly improve C2+ product yields to 21% (from 16% for single bed) which we plan to further improve by considering more sequential beds; 3. Outlined development and validation of new generation of DCKM for the OCM process using the high-information content of spatial concentration profiles obtained in part 2. Most importantly, to improve the current DCKM literature by considering surface reactions that result in early H2 formation. Validated DCKM represent highly valuable numerical tools that allow for the prediction of the OCM performance of different reactor configurations operating under a broad range of conditions, e.g. high pressures, porous wall reactors etc. Consequently, this new generation of comprehensive DCKM based on the sampling profiles, detailed in this report, will be of considerable use in improving the yields of useful products in the OCM process; 4. Explore novel conditions that include oxygen-feed distributed packed bed OCM reactors and coupled catalytic and non-thermal plasma OCM reactors, again to further push the yields for useful C2+ products. The details of the proposed approach for implementing such reactor configurations and development of a new generation of DCKM for the OCM process is outlined in the future work, Chapter 4, of section 1 of the report. Section 2: Direct catalytic conversion of carbon dioxide to liquid fuels and basic chemicals, such as methanol, using solar-derived hydrogen at or near ambient pressure is a highly desirable goal in heterogeneous catalysis. When realized, this technology will pave the way for a sustainable society together with decentralized power generation. Here we report a novel class of holmium (Ho) containing multi-metal oxide Cu catalysts discovered through the application of high-throughput methods. In particular, ternary systems of Cu-GaOx-HoOy > Cu-CeOx-HoOy ~ Cu-LaOx-HoOy supported on -Al2O3 exhibited superior methanol production (10x) with less CO formation than previously reported catalysts at atmospheric pressure. Holmium was shown to be highly dispersed as few-atom clusters, suggesting that the formation of tri-metallic sites could be the key for the promotion of methanol synthesis by Ho.
Author: George Nicolas Kastanas
Publisher:
ISBN:
Category :
Languages : en
Pages : 217
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design strategies that would improve the yields of the useful intermediate products.
Author: Ali khansa
Publisher:
ISBN:
Category : Catalysis
Languages : en
Pages : 60
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Author: Hope O. Otor
Publisher:
ISBN:
Category : Carbon dioxide mitigation
Languages : en
Pages : 210
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Book Description
The anthropogenic emissions of CO2 from industrial processes are considered the major cause of global warming and ocean acidification. To this end, different abatement strategies have been sought to capture CO2 directly from various effluent sources. Carbon capture and sequestration (CCS) have been touted to solve this problem; however, due to the challenges associated with this approach, research efforts have been focused on the development of Dual Function Materials (DFMs) that can effectively capture and convert CO2 to value-added products. To effectively develop a DFM, it is necessary to produce a highly active and stable catalytic material first. The first part of this thesis focuses on the synthesis and characterization of a highly dispersed inverse CeOx-Cu/SiO2 catalyst. Characterization techniques, such as X-ray photoelectron spectroscopy (XPS), N2O chemisorption, and scanning transmission electron microscopy (STEM) analysis revealed effective ceria deposition over the SiO2-supported Cu nanoparticles, which is intended to create a high number of interfacial sites active for the synthesis of methanol from CO2. As Cu catalysts are prone to deactivation, the second part of this thesis is focused on the development of a wet chemical method for encapsulation of the catalyst for control of its deactivation. The alumina overcoating layer proved to be successful in improving the stability of the Cu catalyst under liquid and gas phase conditions.
Author:
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ISBN:
Category :
Languages : en
Pages :
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Author: Mingchen Tang
Publisher:
ISBN: 9781321063387
Category : Carbon dioxide
Languages : en
Pages : 59
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People are increasingly interested in CO2 reforming of CH 4 since the reaction can convert two cheap and abundant greenhouse gases (CH4 and CO2) to useful syngas (H2 +CO). The major challenge of this highly endothermic reforming reaction is carbon deposition and sintering of catalyst, which results in catalyst deactivation and even the blockage of reactor flow path. Ni-based catalysts are considered to be more industrially favorable for the application of CO2 reforming of CH4 reaction because of its ability in reducing the activation energy of the reaction, high availability and low cost; although it is more sensitive to coke formation than noble metals since it can catalyze carbon formation via methane decomposition and the Boudouard reaction. Ni/ZSM-5 catalysts with Ce modification prepared via incipient wetness impregnation method and characterized with BET, XRD, and SEM techniques were used to overcome the challenge. Factorial tests were conducted to evaluate the effects of Ce on the catalytic reforming reaction. Experimental results show that Ce is an effective promoter for the reaction. It can not only improve the selectivity of H 2 in syngas production but also suppress the carbon formation.
