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Title: High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers

Abstract

From the crystal structures of reaction centers (RCs) from purple photosynthetic bacteria, two pathways for electron transfer (ET) are apparent but only one pathway (the A side) operates in the native protein-cofactor complex. Partial activation of the B-side pathway has unveiled the true inefficiencies of ET processes on that side in comparison to analogous reactions on the A side. Of significance are the relative rate constants for forward ET and the competing charge recombination reactions. On the B side, these rate constants are nearly equal for the secondary charge-separation step (ET from bacteriopheophytin to quinone), relegating the yield of this process to < 50%. Herein we report efforts to optimize this step. In surveying all possible residues at position 131 in the M subunit, we discovered that when glutamic acid replaces the native valine the efficiency of the secondary ET is nearly two-fold higher than in the wild-type RC. The positive effect of M131 Glu is likely due to formation of a hydrogen bond with the ring V keto group of the B-side bacteriopheophytin leading to stabilization of the charge-separated state involving this cofactor. In conclusion, this change slows charge recombination by roughly a factor of two and affords themore » improved yield of the desired forward ET to the B-side quinone terminal acceptor.« less

Authors:
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Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1225100
Alternate Identifier(s):
OSTI ID: 1222397; OSTI ID: 1225368
Grant/Contract Number:  
FG-02-09ER16116; AC02-06CH11357; FG02-09ER16116; DGE-1143954
Resource Type:
Published Article
Journal Name:
Biochimica et Biophysica Acta - Bioenergetics
Additional Journal Information:
Journal Name: Biochimica et Biophysica Acta - Bioenergetics Journal Volume: 1837 Journal Issue: 11; Journal ID: ISSN 0005-2728
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; photosynthetic reaction center; charge recombination; high-throughput screening; ultrafast spectroscopy; directed evolution; transmembrane electron transfer

Citation Formats

Kressel, Lucas, Faries, Kaitlyn M., Wander, Marc J., Zogzas, Charles E., Mejdrich, Rachel J., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., and Kirmaier, Christine. High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers. Netherlands: N. p., 2014. Web. doi:10.1016/j.bbabio.2014.07.015.
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Kressel, Lucas, Faries, Kaitlyn M., Wander, Marc J., Zogzas, Charles E., Mejdrich, Rachel J., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., & Kirmaier, Christine. High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers. Netherlands. https://doi.org/10.1016/j.bbabio.2014.07.015
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Kressel, Lucas, Faries, Kaitlyn M., Wander, Marc J., Zogzas, Charles E., Mejdrich, Rachel J., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., and Kirmaier, Christine. Sat . "High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers". Netherlands. https://doi.org/10.1016/j.bbabio.2014.07.015.
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@article{osti_1225100,
title = {High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers},
author = {Kressel, Lucas and Faries, Kaitlyn M. and Wander, Marc J. and Zogzas, Charles E. and Mejdrich, Rachel J. and Hanson, Deborah K. and Holten, Dewey and Laible, Philip D. and Kirmaier, Christine},
abstractNote = {From the crystal structures of reaction centers (RCs) from purple photosynthetic bacteria, two pathways for electron transfer (ET) are apparent but only one pathway (the A side) operates in the native protein-cofactor complex. Partial activation of the B-side pathway has unveiled the true inefficiencies of ET processes on that side in comparison to analogous reactions on the A side. Of significance are the relative rate constants for forward ET and the competing charge recombination reactions. On the B side, these rate constants are nearly equal for the secondary charge-separation step (ET from bacteriopheophytin to quinone), relegating the yield of this process to < 50%. Herein we report efforts to optimize this step. In surveying all possible residues at position 131 in the M subunit, we discovered that when glutamic acid replaces the native valine the efficiency of the secondary ET is nearly two-fold higher than in the wild-type RC. The positive effect of M131 Glu is likely due to formation of a hydrogen bond with the ring V keto group of the B-side bacteriopheophytin leading to stabilization of the charge-separated state involving this cofactor. In conclusion, this change slows charge recombination by roughly a factor of two and affords the improved yield of the desired forward ET to the B-side quinone terminal acceptor.},
doi = {10.1016/j.bbabio.2014.07.015},
journal = {Biochimica et Biophysica Acta - Bioenergetics},
number = 11,
volume = 1837,
place = {Netherlands},
year = {Sat Nov 01 00:00:00 EDT 2014},
month = {Sat Nov 01 00:00:00 EDT 2014}
}
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https://doi.org/10.1016/j.bbabio.2014.07.015
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