De Novo Design of Ln(III) Coiled Coils for Imaging Applications

Berwick, Matthew R.; Lewis, David J.; Jones, Andrew W.; Parslow, Rosemary A.; Dafforn, Timothy R.; Cooper, Helen J.; Wilkie, John; Pikramenou, Zoe; Britton, Melanie M.; Peacock, Anna F. A.

doi:10.1021/ja408741h

Cited by 56 publications

(68 citation statements)

References 30 publications

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“…The r 1 value of our peptide-Gd(III) complexes (Nap-GFFYGRGD-Gd(III) and Nap-GFFYGRGE-Gd(III) complexes) was about 10.4 and 13.7 times that of Magnevist. To the best of our knowledge, these values were the biggest ones for peptide-Gd(III) complexes34243484950. Such a huge enhancement was due to the binding of Gd(III) to the nanofibers and the formation of complexes between Gd(III) and the peptides.…”

Section: Resultsmentioning

confidence: 80%

“…Inspired by nature, researchers have developed many biofunctional nanomaterials formed by the specific interactions between metal ions and peptides34567. Among them, supramolecular hydrogels89101112, especially those of peptides13141516171819202122232425, have attracted research interests due to their inherent biocompatibility, degradability, and fast responsiveness to external stimuli26272829303132.…”

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confidence: 99%

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Gd(III)-induced Supramolecular Hydrogelation with Enhanced Magnetic Resonance Performance for Enzyme Detection

Hua

et al. 2017

Sci Rep

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Here we report a supramolecular hydrogel based on Gd(III)-peptide complexes with dramatically enhanced magnetic resonance (MR) performance. The hydrogelations were formed by adding Gd(III) ion to the nanofiber dispersion of self-assembling peptides naphthalene-Gly-Phe-Phe-Tyr-Gly-Arg-Gly-Asp (Nap-GFFYGRGD) or naphthalene-Gly-Phe-Phe-Tyr-Gly-Arg-Gly-Glu (Nap-GFFYGRGE). We further showed that, by adjusting the molar ratio between Gd(III) and the corresponding peptide, the mechanical property of resulting gels could be fine-tuned. The longitudinal relaxivity (r1) of the Nap-GFFYGRGE-Gd(III) was 58.9 mM−1 S−1, which to our knowledge is the highest value for such peptide-Gd(III) complexes so far. Such an enhancement of r1 value could be applied for enzyme detection in aqueous solutions and cell lysates.

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Section: Resultsmentioning

confidence: 80%

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confidence: 99%

Gd(III)-induced Supramolecular Hydrogelation with Enhanced Magnetic Resonance Performance for Enzyme Detection

Hua

et al. 2017

Sci Rep

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“…Performing the same pH CD titration for a buried Tb(III) binding site, as featured in MB1-2, should show a notable change in folding on de-complexation. 8,9 Though the CD pH titration shows a steady decrease in MB1-2 folding as a function of pH, see Fig. S5B, † it is not consistent with full Tb(III) de-complexation and complete conversion to the apo form, which is only 21 ± 3% folded at pH 7.…”

Section: Ph Dependence Of Tb(iii) Binding To Single Site Peptidesmentioning

confidence: 90%

pH dependent binding in de novo hetero bimetallic coiled coils

et al. 2018

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a Herein the first example of a bimetallic coiled coil featuring a lanthanide binding site is reported, opening opportunities to exploit the attractive NMR and photophysical properties of the lanthanides in multi metallo protein design. In our efforts to fully characterise the system we identified for the first time that lanthanide binding to such sites is pH dependent, with optimal binding at neutral pH, and that the double AsnAsp site is more versatile in this regard than the single Asp site. Our second site featured the structural HgCys 3 site, the chemistry of which was essentially unaltered by the presence of the lanthanide site. In fact, both metal binding sites within the hetero bimetallic coiled coil displayed the same properties as their mononuclear single binding site controls, and operated independently of each other. Finally, pH can be used as an external trigger to control the binding of Hg(II) and Tb(III) to the two distinct sites within this coiled coil, and offers the opportunity to "activate" metal binding sites within complex multi metallo and multi-functional designs.

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“…In particular, the unquenched orbital moment of Eu(III) with the 7 F 0 ground state can give rise to fascinating magnetic properties associated with its anisotropy. Therefore, Ln(III) complexes may be applicable to the in vivo contrast imaging and luminescent probes [19][20][21][22][23][24]. To date, the magnetic properties of the Ln(III) complexes with homoleptic DBM, and mixed DBM and phen have not been reported.…”

Section: Introductionmentioning

confidence: 99%