KUKU

KU ScholarWorks

  • myKU
  • Email
  • Enroll & Pay
  • KU Directory
    • Login
    View Item 
    •   KU ScholarWorks
    • Dissertations and Theses
    • Dissertations
    • View Item
    •   KU ScholarWorks
    • Dissertations and Theses
    • Dissertations
    • View Item
    JavaScript is disabled for your browser. Some features of this site may not work without it.

    Design and Fundamental Understanding of Novel Catalysts for Efficient Transformations of Shale Gas Components

    Thumbnail
    View/Open
    Li_ku_0099D_17251_DATA_1.pdf (7.721Mb)
    Issue Date
    2020-08-31
    Author
    Li, Yuting
    Publisher
    University of Kansas
    Format
    232 pages
    Type
    Dissertation
    Degree Level
    Ph.D.
    Discipline
    Chemical & Petroleum Engineering
    Rights
    Copyright held by the author.
    Metadata
    Show full item record
    Abstract
    In recent years, due to the abundant storage and development of hydraulic techniques, studies relating to the inexpensive shale gas source have drawn increasing attention among both academic and industrial researchers. Besides the utilization in heating and electricity of ordinary life, the more important application of shale gas is to be used as the raw carbon source in the chemical industry. As a chemical feedstock, it can be converted to various value-added intermediates, such as oxygenates, olefins and heavy hydrocarbons, via distinct catalytic processes. In this dissertation, there are five significant catalytic processes discussed in detail, including the one-step production of acetic acid by coupling methane with carbon monoxide and oxygen under mild conditions, the complete oxidation of methane at relatively low temperature, the oxidation of ethane to form carboxylic acids (acetic acid and formic acid) at near room temperature and near ambient pressure, the stable dehydrogenation of ethane to produce ethylene, and the synthesis of formic acid directly from carbon monoxide at low temperature. To improve the efficiency of these catalytic transformations, the design of novel catalysts exhibiting good activity of the activation of methane or ethane and high selectivity of the ideal product is the key. Thus, a variety of novel catalysts were prepared through different synthetic methodologies and were used in these catalytic transformations of short-chain alkanes. Specifically, the singly dispersed rhodium atoms anchored in microporous aluminosilicate materials were employed for the effective conversion of methane and ethane into acetic acid that is one of the most significant chemical materials due to its wide applications. In addition, the coordination-number dependent nickel oxide catalysts were applied in the complete oxidation of methane at relatively low temperatures. Moreover, Pd promoted Zn-based catalysts were used for the enhancement of activity and stability of the production of olefin from ethane dehydrogenation. Furthermore, the new type of the zeolitic material - nanosheet FAU catalysts, synthesized by using the graphene oxide with confined spaces as a special template, were utilized to produce formic acid from carbon monoxide, which could be formed from methane, reacting with water at low temperature. As these proposed catalysts presented good performances of the listed catalytic transformations, it is essential to know how these catalysts activate methane or ethane and convert them into ideal products. In this dissertation, fundamental understandings of authentic structures of synthesized catalysts at an atomic level were obtained by using the multiple ex-situ and in-situ characterization techniques. Through the integration of the fundamental understanding of local structures of these catalysts under catalytic conditions and the experimental explorations of their catalytic performances, the correlation between the structure of catalysts and their activities can be built. The establishment of such intrinsic structure-activity correlation is meaningful for the advances of new types of catalysts in science and is beneficial to the future realization of feasible processes. To conclude, investigations in this dissertation demonstrated the design and fundamental understanding of novel catalysts for efficient transformations of shale gas components under relatively mild conditions. The applied methodologies and achieved results in these studies will provide insights into both essential studies and practical processes involving the activation and conversion of light hydrocarbons (methane and ethane).
    URI
    http://hdl.handle.net/1808/32600
    Collections
    • Dissertations [4475]

    Items in KU ScholarWorks are protected by copyright, with all rights reserved, unless otherwise indicated.


    We want to hear from you! Please share your stories about how Open Access to this item benefits YOU.


    Contact KU ScholarWorks
    785-864-8983
    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    785-864-8983

    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    Image Credits
     

     

    Browse

    All of KU ScholarWorksCommunities & CollectionsThis Collection

    My Account

    LoginRegister

    Statistics

    View Usage Statistics

    Contact KU ScholarWorks
    785-864-8983
    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    785-864-8983

    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    Image Credits
     

     

    The University of Kansas
      Contact KU ScholarWorks
    Lawrence, KS | Maps
     
    • Academics
    • Admission
    • Alumni
    • Athletics
    • Campuses
    • Giving
    • Jobs

    The University of Kansas prohibits discrimination on the basis of race, color, ethnicity, religion, sex, national origin, age, ancestry, disability, status as a veteran, sexual orientation, marital status, parental status, gender identity, gender expression and genetic information in the University’s programs and activities. The following person has been designated to handle inquiries regarding the non-discrimination policies: Director of the Office of Institutional Opportunity and Access, IOA@ku.edu, 1246 W. Campus Road, Room 153A, Lawrence, KS, 66045, (785)864-6414, 711 TTY.

     Contact KU
    Lawrence, KS | Maps