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    Development of Reusable heterogeneous Catalysts for Sustainable formic acid production and methanol utilization

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    Thesis_V6_20190318.docx.pdf
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    PDF
    Description:
    Ding-Jier Yuan - Final Paper Submission
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    Type
    Dissertation
    Authors
    Yuan, Ding-Jier cc
    Advisors
    Huang, Kuo-Wei cc
    Committee members
    Han, Yu cc
    Lai, Zhiping cc
    Yang, Arnold Chang-Mou
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2019-02
    Embargo End Date
    2021-04-01
    Permanent link to this record
    http://hdl.handle.net/10754/631817
    
    Metadata
    Show full item record
    Access Restrictions
    At the time of archiving, the student author of this dissertation opted to temporarily restrict access to it. The full text of this dissertation became available to the public after the expiration of the embargo on 2021-04-01.
    Abstract
    The green production of formic acid and utilization of methanol over heterogeneous catalysis system were investigated in this study. The heterogeneous catalysts are widely used in the chemical industry. They offer high stability and reusability which can enhance the production ability and lower the production cost, it can be considered as the sustainable energy solution for the future. In this work, we demonstrated several different heterogeneous catalysts for sustainable formic acid production and methanol utilization, including the heteropoly acid supported mesoporous silica catalysts and multi-function mixed metal oxide catalysts. Detailed characterizations of the final products were carried out by N2 adsorption and desorption, XRD, HR-TEM, SEM, ICP-OES, XANES, NH3- TPD, Raman spectroscopy, and FTIR to identify the chemical properties and physical properties of the catalysts. We obtained 60 % glycerol conversion and 30 % formic acid selectivity with at least 3 rounds of usages in batch system over PV1Mo/SBA-15-p-DS catalyst. Moreover, the continuous methyl formate production with significantly high formation rate (16.7) has been achieved via our CuMgO-based catalysts, and the best Cu5MgO5 catalyst gives more than 80 % methanol conversion with constant selectivity to methyl formate even after 4 catalytic test (more than 200 h), revealing their potential for industrialization. For the methanol utilization reaction, the methanol homocoupling to form dimethoxymethane (DMM) has been investigated. The redox and acidic properties of catalysts both play a critical role in this reaction and the related to different product. The supported V2O5 catalyst achieves the best catalytic performance (62.1 % conversion and 85.6 % DMM selectivity) with a Ce/Al specific ratio of 1. This research not only provided the efficient catalysts for numerous application with high activity, but also discovered the relation between the catalytic performance and the nature of the materials. These findings might further help the researcher to solve the global environmental and energy issues in the near future.
    Citation
    Yuan, D.-J. (2019). Development of Reusable heterogeneous Catalysts for Sustainable formic acid production and methanol utilization. KAUST Research Repository. https://doi.org/10.25781/KAUST-68241
    DOI
    10.25781/KAUST-68241
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-68241
    Scopus Count
    Collections
    PhD Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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