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Title: NADPH-dependent sulfite reductase flavoprotein adopts an extended conformation unique to this diflavin reductase

Abstract

This is the first X-ray crystal structure of the monomeric form of sulfite reductase (SiR) flavoprotein (SiRFP-60) that shows the relationship between its major domains in an extended position not seen before in any homologous diflavin reductases. Small angle neutron scattering confirms this novel domain orientation also occurs in solution. Activity measurements of SiR and SiRFP variants allow us to propose a novel mechanism for electron transfer from the SiRFP reductase subunit to its oxidase metalloenzyme partner that, together, make up the SiR holoenzyme. Specifically, we propose that SiR performs its 6-electron reduction via intramolecular or intermolecular electron transfer. Furthermore, our model explains both the significance of the stoichiometric mismatch between reductase and oxidase subunits in the holoenzyme and how SiR can handle such a large volume electron reduction reaction that is at the heart of the sulfur bio-geo cycle.

Authors:
 [1];  [1];  [2];  [1];  [1]; ORCiD logo [3];  [1]
  1. Dept. of Biological Science and Institute of Molecular Biophysics, Tallahassee, FL (United States)
  2. Dept. of Biological Science and Institute of Molecular Biophysics, Tallahassee, FL (United States); Univ. of Wisconsin, Madison, WI (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1545231
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Structural Biology
Additional Journal Information:
Journal Volume: 205; Journal Issue: 2; Journal ID: ISSN 1047-8477
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; Flavoprotein; Diflavin reductase; Cytochrome p450 reductase; Electron transfer; X-ray crystallography; SANS

Citation Formats

Tavolieri, Angela M., Murray, Daniel T., Askenasy, Isabel, Pennington, Joseph M., McGarry, Lauren, Stanley, Christopher B., and Stroupe, Margaret Elizabeth. NADPH-dependent sulfite reductase flavoprotein adopts an extended conformation unique to this diflavin reductase. United States: N. p., 2019. Web. doi:10.1016/j.jsb.2019.01.001.
Tavolieri, Angela M., Murray, Daniel T., Askenasy, Isabel, Pennington, Joseph M., McGarry, Lauren, Stanley, Christopher B., & Stroupe, Margaret Elizabeth. NADPH-dependent sulfite reductase flavoprotein adopts an extended conformation unique to this diflavin reductase. United States. https://doi.org/10.1016/j.jsb.2019.01.001
Tavolieri, Angela M., Murray, Daniel T., Askenasy, Isabel, Pennington, Joseph M., McGarry, Lauren, Stanley, Christopher B., and Stroupe, Margaret Elizabeth. Tue . "NADPH-dependent sulfite reductase flavoprotein adopts an extended conformation unique to this diflavin reductase". United States. https://doi.org/10.1016/j.jsb.2019.01.001. https://www.osti.gov/servlets/purl/1545231.
@article{osti_1545231,
title = {NADPH-dependent sulfite reductase flavoprotein adopts an extended conformation unique to this diflavin reductase},
author = {Tavolieri, Angela M. and Murray, Daniel T. and Askenasy, Isabel and Pennington, Joseph M. and McGarry, Lauren and Stanley, Christopher B. and Stroupe, Margaret Elizabeth},
abstractNote = {This is the first X-ray crystal structure of the monomeric form of sulfite reductase (SiR) flavoprotein (SiRFP-60) that shows the relationship between its major domains in an extended position not seen before in any homologous diflavin reductases. Small angle neutron scattering confirms this novel domain orientation also occurs in solution. Activity measurements of SiR and SiRFP variants allow us to propose a novel mechanism for electron transfer from the SiRFP reductase subunit to its oxidase metalloenzyme partner that, together, make up the SiR holoenzyme. Specifically, we propose that SiR performs its 6-electron reduction via intramolecular or intermolecular electron transfer. Furthermore, our model explains both the significance of the stoichiometric mismatch between reductase and oxidase subunits in the holoenzyme and how SiR can handle such a large volume electron reduction reaction that is at the heart of the sulfur bio-geo cycle.},
doi = {10.1016/j.jsb.2019.01.001},
journal = {Journal of Structural Biology},
number = 2,
volume = 205,
place = {United States},
year = {Tue Jan 15 00:00:00 EST 2019},
month = {Tue Jan 15 00:00:00 EST 2019}
}

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