Development of electronic structure and kinetics methods for the rational design of electrocatalysts
Name
1142099325-MIT.pdf
Size
11.83 MB
Format
Adobe PDF
Checksum (MD5)
b07bda71c2808c3c48e0ece8fd16e63e
Author(s)
Ricke, Nathan Darrell Peterson.
Advisor(s)
Troy Van Voorhis.
Date Issued
2019
Publisher
Massachusetts Institute of Technology
Abstract
Computational modeling has untapped potential for novel material and chemical discovery. In this thesis, we explore ways to improve existing modeling methods, and how to apply these methods to design novel graphite-conjugated catalysts (GCCs). For improving electronic structure methods, we first present an extended study of bootstrap embedding theory (BET) and its ability to recover static correlation, as well as a proof on BET's ideal convergence properties. We then present a theoretical analysis using density functional theory (DFT) on a class of GCCs containing cationic nitrogen atoms, which are particularly active for catalyzing the oxygen reduction reaction (ORR). Using a mixture of high-throughput screening, statistical analysis, and computational exploration guided by chemical intuition, we design several novel GCCs, several of which DFT predicts would have enhanced activity above existing GCCs. Furthermore, our analysis reveals that known ORR scaling relations hold for GCCs, but hint at the possibility of breaking these relations with careful molecular engineering of the GCC active sites.
Description
Thesis: Ph. D., Massachusetts Institute of Technology, Department of Chemistry, 2019
Cataloged from PDF version of thesis.
Includes bibliographical references (pages 79-87).
Subjects
Chemistry.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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