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Mathematical Modeling of Ammonia Electro-Oxidation on Polycrystalline Pt Deposited Electrodes

Diaz Aldana, Luis A.
http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1395077873

Abstract Details

2014, Doctor of Philosophy (PhD), Ohio University, Chemical Engineering (Engineering and Technology).
The ammonia electrolysis process has been proposed as a feasible way for electrochemical generation of fuel grade hydrogen (H2). Ammonia is identified as one of the most suitable energy carriers due to its high hydrogen density, and its safe and efficient distribution chain. Moreover, the fact that this process can be applied even at low ammonia concentration feedstock opens its application to wastewater treatment along with H2 co-generation. In the ammonia electrolysis process, ammonia is electro-oxidized in the anode side to produce N2 while H2 is evolved from water reduction in the cathode. A thermodynamic energy requirement of just five percent of the energy used in hydrogen production from water electrolysis is expected from ammonia electrolysis. However, the absence of a complete understanding of the reaction mechanism and kinetics involved in the ammonia electro-oxidation has not yet allowed the full commercialization of this process. For that reason, a kinetic model that can be trusted in the design and scale up of the ammonia electrolyzer needs to be developed. This research focused on the elucidation of the reaction mechanism and kinetic parameters for the ammonia electro-oxidation. The definition of the most relevant elementary reactions steps was obtained through the parallel analysis of experimental data and the development of a mathematical model of the ammonia electro-oxidation in a well defined hydrodynamic system, such as the rotating disk electrode (RDE). Ammonia electro-oxidation to N2 as final product was concluded to be a slow surface confined process where parallel reactions leading to the deactivation of the catalyst are present. Through the development of this work it was possible to define a reaction mechanism and values for the kinetic parameters for ammonia electro-oxidation that allow an accurate representation of the experimental observations on a RDE system. Additionally, the validity of the reaction mechanism and kinetic parameters were supplemented by means of process scale up, performance evaluation, and hydrodynamic analysis in a flow cell electrolyzer. An adequate simulation of the flow electrolyzer performance was accomplished using the obtained kinetic parameters.
Gerardine Botte, Ph.D. (Advisor)
Valerie Young, Ph.D. (Committee Member)
Gang Chen, Ph.D. (Committee Member)
Savas Kaya, Ph.D. (Committee Member)
Howard Dewald, Ph.D. (Committee Member)
211 p.
Chemical Engineering; Chemistry; Energy; Engineering
Ammonia Electro-Oxidation; Mathematical Modeling; Electrolyzer; Polycrystalline Platinum; Reaction Mechanism; Kinetic Parameters; Hydrodynamic Analysis

Recommended Citations

Citations

  • Diaz Aldana, L. A. (2014). Mathematical Modeling of Ammonia Electro-Oxidation on Polycrystalline Pt Deposited Electrodes [Doctoral dissertation, Ohio University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1395077873

    APA Style (7th edition)

  • Diaz Aldana, Luis. Mathematical Modeling of Ammonia Electro-Oxidation on Polycrystalline Pt Deposited Electrodes. 2014. Ohio University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1395077873.

    MLA Style (8th edition)

  • Diaz Aldana, Luis. "Mathematical Modeling of Ammonia Electro-Oxidation on Polycrystalline Pt Deposited Electrodes." Doctoral dissertation, Ohio University, 2014. http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1395077873

    Chicago Manual of Style (17th edition)

ohiou1395077873
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© 2014, all rights reserved.
This open access ETD is published by Ohio University and OhioLINK.