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David"]},{"label":"Held By","value":"Wesleyan University Library, Wesleyan University, Middletown, CT, USA"},{"label":"Genre","value":["theses"]},{"label":"Name(s)","value":["Majaducon, Leonard Vincent Anona (creator)"]},{"label":"Administrative Note","value":"Drupal Node ID: 48562<br>author email: lmajaducon@wesleyan.edu<br>old filename: 1239_379144"},{"label":"Author-supplied Keywords","value":["MRI","Chromium(III)","Relaxivity"]},{"label":"Degree","value":["Bachelor of Arts with Departmental Honors"]},{"label":"Description","value":"<p>Our limited understanding of prototropic exchange, its mechanisms, and its role in enhancing magnetic resonance (MR) contrast poses a key challenge in the design and development of next-generation MR imaging contrast agents (CAs). CrIII complexes with the cyclen (1,4,7,10-tetraaza-1,4,7,10-tetracyclododecane) and DOTAM (1,4,7,10-tetraaza-1,4,7,10-tetra(2-carbamoylmethyl)cyclododecane) chelates were studied as models of aquo and amine ([Cr(cyclen)(H2O)2]3+) and amide prototropic exchange ([Cr(DOTAM)]3+), respectively. The contributions of inner sphere, second sphere, outer sphere processes to the observed relaxivity and its relationship with the relaxation process, presented herein as prototropic exchange kinetically-coupled to spin relaxation, are discussed. The pH- and temperature-dependent 1H-relaxometry revealed three prototropic exchange mechanisms in the aquo and amine model: a water-mediated pathway, a hydronium mediated pathway, and a Grotthuss diffusion pathway. Each pathway is operative at different pH conditions, depending on the protonation state of [Cr(cyclen)(H2O)2]3+. Based on the structure and rip profiles of [Cr(cyclen)(H2O)2]3+, we propose herein key considerations to leverage moieties with exchangeable hydroxy and amine protons in the design of CAs. [Cr(DOTAM)]3+ exhibited an rip profile invariant to pH. The DOTAM complex primarily relaxes via outer sphere processes with spin relaxation as the rate-determining step. The relaxometric behavior of these two complexes may extend to other transition metal complexes, particularly those of a non-S type ground state or those that are kinetically inert. The results have potential applications in the development of responsive paraCEST agents.</p>"},{"label":"Group","value":["Theses & Dissertations"]},{"label":"Digital Origin","value":["born digital"]},{"label":"Discipline","value":["Chemistry"]},{"label":"Date","value":"April 15, 2024"},{"label":"EDTF Date","value":"D:00 M:00 Y:2024"},{"label":"File Format","value":["application/pdf"]},{"label":"Digital Object Identifier (DOI)","value":"https://doi.org/10.14418/wes01.1.2941"},{"label":"Type","value":["Text"]}],"description":"Cyclen complexes of Cr(III): Models for prototropic 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