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@ARTICLE{Bolton:1024817,
author = {Bolton, Rachel and Machelett, Moritz M. and Stubbs, Jack
and Axford, Danny and Caramello, Nicolas and Catapano,
Lucrezia and Malý, Martin and Rodrigues, Matthew J. and
Cordery, Charlotte and Tizzard, Graham J. and MacMillan,
Fraser and Engilberge, Sylvain and von Stetten, David and
Tosha, Takehiko and Sugimoto, Hiroshi and Worrall, Jonathan
A. R. and Webb, Jeremy S. and Zubkov, Mike and Coles, Simon
and Mathieu, Eric and Steiner, Roberto A. and Murshudov,
Garib and Schrader, Tobias E. and Orville, Allen M. and
Royant, Antoine and Evans, Gwyndaf and Hough, Michael A. and
Owen, Robin L. and Tews, Ivo},
title = {{A} redox switch allows binding of {F}e({II}) and
{F}e({III}) ions in the cyanobacterial iron-binding protein
{F}ut{A} from {P}rochlorococcus},
journal = {Proceedings of the National Academy of Sciences of the
United States of America},
volume = {121},
number = {12},
issn = {0027-8424},
address = {Washington, DC},
publisher = {National Acad. of Sciences},
reportid = {FZJ-2024-02483},
pages = {e2308478121},
year = {2024},
abstract = {The marine cyanobacterium Prochlorococcus is a main
contributor to global photosynthesis, whilst being limited
by iron availability. Cyanobacterial genomes generally
encode two different types of FutA iron-binding proteins:
periplasmic FutA2 ABC transporter subunits bind Fe(III),
while cytosolic FutA1 binds Fe(II). Owing to their small
size and their economized genome Prochlorococcus ecotypes
typically possess a single futA gene. How the encoded FutA
protein might bind different Fe oxidation states was
previously unknown. Here, we use structural biology
techniques at room temperature to probe the dynamic behavior
of FutA. Neutron diffraction confirmed four negatively
charged tyrosinates, that together with a neutral water
molecule coordinate iron in trigonal bipyramidal geometry.
Positioning of the positively charged Arg103 side chain in
the second coordination shell yields an overall
charge-neutral Fe(III) binding state in structures
determined by neutron diffraction and serial femtosecond
crystallography. Conventional rotation X-ray crystallography
using a home source revealed X-ray-induced photoreduction of
the iron center with observation of the Fe(II) binding
state; here, an additional positioning of the Arg203 side
chain in the second coordination shell maintained an overall
charge neutral Fe(II) binding site. Dose series using serial
synchrotron crystallography and an XFEL X-ray pump–probe
approach capture the transition between Fe(III) and Fe(II)
states, revealing how Arg203 operates as a switch to
accommodate the different iron oxidation states. This
switching ability of the Prochlorococcus FutA protein may
reflect ecological adaptation by genome streamlining and
loss of specialized FutA proteins.},
cin = {JCNS-FRM-II / JCNS-4 / MLZ},
ddc = {500},
cid = {I:(DE-Juel1)JCNS-FRM-II-20110218 /
I:(DE-Juel1)JCNS-4-20201012 / I:(DE-588b)4597118-3},
pnm = {6G4 - Jülich Centre for Neutron Research (JCNS) (FZJ)
(POF4-6G4) / 632 - Materials – Quantum, Complex and
Functional Materials (POF4-632)},
pid = {G:(DE-HGF)POF4-6G4 / G:(DE-HGF)POF4-632},
experiment = {EXP:(DE-MLZ)BIODIFF-20140101},
typ = {PUB:(DE-HGF)16},
pubmed = {38489389},
UT = {WOS:001206418700003},
doi = {10.1073/pnas.2308478121},
url = {https://juser.fz-juelich.de/record/1024817},
}