Force-induced chemical reactions on the metal centre in a single metalloprotein molecule

Peng Zheng, Guilherme M. Arantes (), Martin J. Field and Hongbin Li ()
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Peng Zheng: University of British Columbia
Guilherme M. Arantes: Instituto de Química, Universidade de São Paulo
Martin J. Field: Institut de Biologie Structurale (IBS) Jean-Pierre Ebel, CEA/CNRS/Universite Joseph Fourier
Hongbin Li: University of British Columbia

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Metalloproteins play indispensable roles in biology owing to the versatile chemical reactivity of metal centres. However, studying their reactivity in many metalloproteins is challenging, as protein three-dimensional structure encloses labile metal centres, thus limiting their access to reactants and impeding direct measurements. Here we demonstrate the use of single-molecule atomic force microscopy to induce partial unfolding to expose metal centres in metalloproteins to aqueous solution, thus allowing for studying their chemical reactivity in aqueous solution for the first time. As a proof-of-principle, we demonstrate two chemical reactions for the FeS4 centre in rubredoxin: electrophilic protonation and nucleophilic ligand substitution. Our results show that protonation and ligand substitution result in mechanical destabilization of the FeS4 centre. Quantum chemical calculations corroborated experimental results and revealed detailed reaction mechanisms. We anticipate that this novel approach will provide insights into chemical reactivity of metal centres in metalloproteins under biologically more relevant conditions.

Date: 2015
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DOI: 10.1038/ncomms8569

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