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Engineering Synthetic Electron Transfer Chains from Metallopeptide Membranes.
Inorg Chem
February 2024
Department of Chemistry, Trinity University, San Antonio, Texas 78212, United States.
The energetic and geometric features enabling redox chemistry across the copper cupredoxin fold contain key components of electron transfer chains (ETC), which have been extended here by templating the cross-β bilayer assembly of a synthetic nonapeptide, HHQALVFFA-NH (K16A), with copper ions. Similar to ETC cupredoxin plastocyanin, these assemblies contain copper sites with blue-shifted ( 573 nm) electronic transitions and strongly oxidizing reduction potentials. Electron spin echo envelope modulation and X-ray absorption spectroscopies define square planar Cu(II) sites containing a single His ligand.
View Article and Find Full Text PDFCyclic Ruthenium-Peptide Conjugates as Integrin-Targeting Phototherapeutic Prodrugs for the Treatment of Brain Tumors.
J Am Chem Soc
July 2023
Leiden Institute of Chemistry, Universiteit Leiden, Einsteinweg 55, 2333 CC Leiden, Netherlands.
To investigate the potential of tumor-targeting photoactivated chemotherapy, a chiral ruthenium-based anticancer warhead, Λ/Δ-[Ru(Phphen)(OH)], was conjugated to the RGD-containing Ac-MRGDH-NH peptide by direct coordination of the M and H residues to the metal. This design afforded two diastereoisomers of a cyclic metallopeptide, Λ-[]Cl and Δ-[]Cl. In the dark, the ruthenium-chelating peptide had a triple action.
View Article and Find Full Text PDFHistidine Ligated Iron-Sulfur Peptides.
Chembiochem
July 2022
D-CIBIO, University of Trento, via Sommarive 9, 38123, Trento 28123, Italy.
Iron-sulfur clusters are thought to be ancient cofactors that could have played a role in early protometabolic systems. Thus far, redox active, prebiotically plausible iron-sulfur clusters have always contained cysteine ligands to the cluster. However, extant iron-sulfur proteins can be found to exploit other modes of binding, including ligation by histidine residues, as seen with [2Fe-2S] Rieske and MitoNEET proteins.
View Article and Find Full Text PDFMacrocylases as synthetic tools for ligand synthesis: enzymatic synthesis of cyclic peptides containing metal-binding amino acids.
R Soc Open Sci
November 2021
EaStCHEM School of Chemistry, University of Edinburgh, Joseph Black Building, David Brewster Rd, Edinburgh EH9 3FJ, Scotland.
Improving the sustainability of synthesis is a major goal in green chemistry, which has been greatly aided by the development of asymmetric transition metal catalysis. Recent advances in asymmetric catalysis show that the ability to control the coordination sphere of substrates can lead to improvements in enantioselectivity and activity, in a manner resembling the operation of enzymes. Peptides can be used to mimic enzyme structures and their secondary interactions and they are easily accessible through solid-phase peptide synthesis.
View Article and Find Full Text PDFReinforced Room-Temperature Spin Filtering in Chiral Paramagnetic Metallopeptides.
J Am Chem Soc
October 2020
ICMol, Universitat de València, C/Catedrático José Beltrán no. 2, Paterna, Valencia 46980, Spain.
Chirality-induced spin selectivity (CISS), whereby helical molecules polarize the spin of electrical current, is an intriguing effect with potential applications in nanospintronics. In this nascent field, the study of the CISS effect using paramagnetic chiral molecules, which could introduce another degree of freedom in controlling the spin transport, remains so far unexplored. To address this challenge, herein we propose the use of self-assembled monolayers (SAMs) of helical lanthanide-binding peptides.
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