Super-Resolution Single-Molecule Fluorescence Imaging for Studying Intracellular Transition-Metal Catalysis & Reductive Amination of Carbonyl Compounds Catalyzed by Half-Sandwich Iridium Complexes Under Mild Reaction Conditions

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dc.contributor.advisorDo, Loi H.
dc.contributor.committeeMemberMiljanić, Ognjen Š.
dc.contributor.committeeMemberChen, Tai-Yen
dc.contributor.committeeMemberLee, T. Randall
dc.contributor.committeeMemberWang, Yuhong
dc.creatorNguyen, Dat Phat
dc.creator.orcid0000-0002-0634-8994
dc.date.accessioned2023-01-18T01:57:51Z
dc.date.createdMay 2022
dc.date.issued2022-04-21
dc.date.updated2023-01-18T01:57:53Z
dc.description.abstractIn recent years, the field of intracellular catalysis has gained much popularity due to the ability of transition-metal complexes to promote selective reactions inside living organisms. Unfortunately, precise quantification of intracellular activity of a metal catalyst cannot be achieved using current ensemble-averaged methods. Instead, we proposed that single-molecule measurement techniques might provide valuable kinetic and mechanistic data that would enhance our understanding of intracellular catalytic behavior. Super-resolution fluorescence microscopy is an advanced optical technique that allows scientists to visualize individual biomolecules inside living cells. This method has been employed to observe and characterize various biological events at a molecular level. We herein describe our work using single-molecule imaging to evaluate the ruthenium-catalyzed uncaging of alloc-protected fluorescent probes inside living cells. This study will allow us to derive important kinetic and biological insights into the intracellular protecting group cleavage process. In the second project, we demonstrated that the conversion of aldehydes and ketones to primary amines could be promoted by half-sandwich iridium complexes using ammonium formate as both the nitrogen and hydride source. The reductive amination of a variety of carbonyl substrates in common polar solvents at 37 °C provided excellent selectivity for the amine over alcohol product. In aqueous media, selective reduction of carbonyls to primary amines was achieved in the absence of acids. Unfortunately, at catalyst concentrations of <1 mM in water, reductive amination efficiency dropped significantly, which suggests that this catalytic methodology might be not suitable for aqueous applications where very low catalyst concentration is required (e.g., inside living cells).
dc.description.departmentChemistry, Department of
dc.format.digitalOriginborn digital
dc.format.mimetypeapplication/pdf
dc.identifier.citationPortions of this document appear in: Nguyen, Dat P., Rudolph N. Sladek, and Loi H. Do. "Scope and limitations of reductive amination catalyzed by half-sandwich iridium complexes under mild reaction conditions." Tetrahedron letters 61, no. 32 (2020): 152196.
dc.identifier.urihttps://hdl.handle.net/10657/13635
dc.language.isoeng
dc.rightsThe author of this work is the copyright owner. UH Libraries and the Texas Digital Library have their permission to store and provide access to this work. UH Libraries has secured permission to reproduce any and all previously published materials contained in the work. Further transmission, reproduction, or presentation of this work is prohibited except with permission of the author(s).
dc.subjectSuper-resolution imaging
dc.subjectSingle-molecule imaging
dc.subjectIntracellular catalysis
dc.subjectAllyl carbamate cleavage
dc.subjectReductive amination
dc.titleSuper-Resolution Single-Molecule Fluorescence Imaging for Studying Intracellular Transition-Metal Catalysis & Reductive Amination of Carbonyl Compounds Catalyzed by Half-Sandwich Iridium Complexes Under Mild Reaction Conditions
dc.type.dcmiText
dc.type.genreThesis
dcterms.accessRightsThe full text of this item is not available at this time because the student has placed this item under an embargo for a period of time. The Libraries are not authorized to provide a copy of this work during the embargo period.
local.embargo.lift2024-05-01
local.embargo.terms2024-05-01
thesis.degree.collegeCollege of Natural Sciences and Mathematics
thesis.degree.departmentChemistry, Department of
thesis.degree.disciplineChemistry
thesis.degree.grantorUniversity of Houston
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy

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