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Title: Selective lanthanide binding sites engineered within a de novo designed coiled coil
Author: Slope, Louise Nicola
ISNI:       0000 0004 6494 852X
Awarding Body: University of Birmingham
Current Institution: University of Birmingham
Date of Award: 2017
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De novo designed coiled coils are described that are capable of selectively discriminating between Ln3+ ions. Sites buried within the hydrophobic core are able to actively discriminate against both larger and smaller ions. Whereas linearly translating the binding site towards the N-terminus, ‘turns-off’ selectivity, owing to N-terminal fraying and flexibility. Mutating first sphere coordinating and second sphere non-coordinating residues was found to impact on the metal coordination chemistry, including the hydration state of the bound Tb3+, which in turn led to altered metal selectivity and MRI relaxivities of the Gd3+ complexes. Given these findings, a novel two binding site coiled coil trimer was designed in which incorporation of both a ‘buried’ and N-terminal site enabled two different Ln3+ ions with differing properties to be bound within a single system. This dual lanthanide binding construct resembles a significant development within the field, being the first example established in a peptide assembly, and is notably even capable of selectively binding and discriminating between two different, but similar, Ln3+ ions. Translating the second Ln3+ binding site linearly along the coiled coil resulted in a series of dual Ln3+ binding peptides in which the distance between the metal ions can be controlled.
Supervisor: Not available Sponsor: Engineering and Physical Sciences Research Council (EPSRC) ; University of Birmingham
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: QD Chemistry