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Understanding Electrochemical Interface Properties by Comprehensive Self-Consistent Density Functional Theory

Zhao, Meng
http://rave.ohiolink.edu/etdc/view?acc_num=case1491315734773944

Abstract Details

2017, Doctor of Philosophy, Case Western Reserve University, Chemistry.
Electrocatalysis gains tremendous attention for recent decades due to its broad applications ranging from electrode sensors to fuel cells and batteries preparations. The fundamental understanding of the electrocatalysis can be obtained by investigating electrochemical properties on the electrode surfaces. Current experimental techniques are unable to characterize the interface at the atomic-scale level in aqueous electrolytes, and theoretical simulations take a role to overcome such limitations. This dissertation utilizes comprehensive self-consistent quantum theory to understand the electrochemical properties of the electrode surfaces. Chapter 1 briefly summarizes the history of theoretical method development in our lab and indicates the overall goal of this dissertation. Chapter 2 demonstrates the step-wise mechanism of electroless Cu deposition on a Cu electrode in the alkaline solution using [Cu(II)EDTA]2- complexes and aldehyde-based reductants. Low-coordinated Cu atoms provided by the surface roughness facilitate C-H bond scission in the reducing agents, producing H(ads), and releasing electrons for Cu(II) reduction. As the electroless Cu deposition process produces hydrogen gas as a byproduct, hydrogen properties on Cu(111) surfaces were explored and discussed in Chapter 3. Chapters 4, 5, and 6 focus on pH-dependent onset potentials of H(ads) and OH(ads) and double layer widths on Pt(111) surface. This fundamental study relates pH, potentials for surface reactions and surface compositions, providing insights into the effects of solution pH on electrochemical properties of the surface. Chapter 7 derives bond dissociation Gibbs energies of R-H bond for adsorbed species, such as CH4(ads), H2O(ads), and HOCH2CH3(ads), on Pt(111) surface from their reversible potentials for bond oxidation, providing a new perspective correlating chemical and electrochemical properties of the adsorbates.
Alfred Anderson (Advisor)
Clemens Burda (Committee Chair)
Daniel Scherson (Committee Member)
John Protasiewicz (Committee Member)
Rohan Akolkar (Committee Member)
206 p.
Chemistry
density functional theory; electrocatalysis; electrochemical surface properties; surface reversible potentials; pH effects

Recommended Citations

Citations

  • Zhao, M. (2017). Understanding Electrochemical Interface Properties by Comprehensive Self-Consistent Density Functional Theory [Doctoral dissertation, Case Western Reserve University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=case1491315734773944

    APA Style (7th edition)

  • Zhao, Meng. Understanding Electrochemical Interface Properties by Comprehensive Self-Consistent Density Functional Theory. 2017. Case Western Reserve University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=case1491315734773944.

    MLA Style (8th edition)

  • Zhao, Meng. "Understanding Electrochemical Interface Properties by Comprehensive Self-Consistent Density Functional Theory." Doctoral dissertation, Case Western Reserve University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=case1491315734773944

    Chicago Manual of Style (17th edition)

case1491315734773944
366
© 2017, all rights reserved.
This open access ETD is published by Case Western Reserve University School of Graduate Studies and OhioLINK.