Reorganization Energy for Internal Electron Transfer in Multicopper Oxidases

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Reorganization Energy for Internal Electron Transfer in Multicopper Oxidases

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Publication Article, peer reviewed scientific
Title Reorganization Energy for Internal Electron Transfer in Multicopper Oxidases
Author(s) Li Hong, Hu ; Farrokhnia, Maryam ; Heimdal, Jimmy ; Shleev, Sergey ; Rulisek, Lubomir ; Ryde, Ulf
Date 2011
English abstract
We have calculated the reorganization energy for the intramolecular electron transfer between the reduced type 1 copper site and the peroxy intermediate of the trinuclear cluster in the multicopper oxidase CueO. The calculations are performed at the combined quantum mechanics and molecular mechanics (QM/MM) level, based on molecular dynamics simulations with tailored potentials for the two copper sites. We obtain a reorganization energy of 91–133 kJ/mol, depending on the theoretical treatment. The two Cu sites contribute by 12 and 22 kJ/mol to this energy, whereas the solvent contribution is 34 kJ/mol. The rest comes from the protein, involving small contributions from many residues. We have also estimated the energy difference between the two electron-transfer states and show that the reduction of the peroxy intermediate is exergonic by 43–87 kJ/mol, depending on the theoretical method. Both the solvent and the protein contribute to this energy difference, especially charged residues close to the two Cu sites. We compare these estimates with energies obtained from QM/MM optimizations and QM calculations in a vacuum and discuss differences between the results obtained at various levels of theory.
DOI http://dx.doi.org/10.1021/jp205897z (link to publisher's fulltext)
Publisher American Chemical Society
Host/Issue Journal of Physical Chemistry B;45
Volume 115
ISSN 1520-5207
Pages 13111-13126
Language eng (iso)
Subject(s) Sciences
Research Subject Categories::NATURAL SCIENCES
Handle http://hdl.handle.net/2043/12853 (link to this page)

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