Control of Heme Coordination and Catalytic Activity by Conformational Changes in Peptide-Amphiphile Assemblies

Journal of the American Chemical Society
Lee A SolomonH Christopher Fry

Abstract

Self-assembling peptide materials have gained significant attention, due to well-demonstrated applications, but they are functionally underutilized. To advance their utility, we use noncovalent interactions to incorporate the biological cofactor heme-B for catalysis. Heme-proteins achieve differing functions through structural and coordinative variations. Here, we replicate this phenomenon by highlighting changes in heme reactivity as a function of coordination, sequence, and morphology (micelles versus fibers) in a series of simple peptide amphiphiles with the sequence c16-xyL3K3-CO2H where c16 is a palmitoyl moiety and xy represents the heme binding region: AA, AH, HH, and MH. The morphology of this peptide series is characterized using transmission electron and atomic force microscopies as well as dynamic light scattering. Within this small library of peptide constructs, we show that three spectroscopically (UV/visible and electron paramagnetic resonance) distinct heme environments were generated: noncoordinated/embedded high-spin, five-coordinate high-spin, and six-coordinate low-spin. The resulting material's functional dependence on sequence and supramolecular morphology is highlighted 2-fold. First, the heme active site ...Continue Reading

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Citations

Mar 30, 2018·Chemical Society Reviews·O ZozuliaI V Korendovych
Aug 7, 2017·Organic & Biomolecular Chemistry·H Christopher FryLee A Solomon
Jun 14, 2018·Chembiochem : a European Journal of Chemical Biology·Giorgio CasertaAngela Lombardi
Feb 23, 2018·Biopolymers·Marco ChinoAngela Lombardi
Mar 5, 2020·Angewandte Chemie·Oleksii Zozulia, Ivan V Korendovych
Apr 25, 2020·Chembiochem : a European Journal of Chemical Biology·Liam R MarshallIvan V Korendovych
Sep 22, 2020·Chembiochem : a European Journal of Chemical Biology·Zsofia Lengyel-ZhandIvan V Korendovych
Feb 3, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Paolo DogniniFrancesca Giuntini
Feb 3, 2021·The Journal of Physical Chemistry. B·H Christopher FryAndrew L Ferguson
Feb 4, 2021·Biochemistry·Areetha D'Souza, Surajit Bhattacharjya
Jan 19, 2021·Chemistry : a European Journal·Oleksii ZozuliaIvan V Korendovych
Apr 13, 2021·Biomacromolecules·Ian W Hamley
Oct 16, 2018·ACS Catalysis·Zsófia LengyelIvan V Korendovych
Dec 10, 2019·Journal of the American Chemical Society·H Christopher FryHannah M Cohn
Jun 8, 2021·Chembiochem : a European Journal of Chemical Biology·Jordon SandlandRoss W Boyle
Sep 15, 2021·Chemical Reviews·Fahmeed SheehanRein V Ulijn

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