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Title: Interprotein electron transfer biohybrid system for photocatalytic H2 production

Abstract

Worldwide there is a large research investment in developing solar fuel systems as clean and sustainable sources of energy. The fundamental mechanisms of natural photosynthesis can provide a source of inspiration for these studies. Photosynthetic reaction center (RC) proteins capture and convert light energy into chemical energy that is ultimately used to drive oxygenic water-splitting and carbon fixation. For the light energy to be used, the RC communicates with other donor/acceptor components via a sophisticated electron transfer scheme that includes electron transfer reactions between soluble and membrane bound proteins. Herein, we reengineer an inherent interprotein electron transfer pathway in a natural photosynthetic system to make it photocatalytic for aqueous H-2 production. The native electron shuttle protein ferredoxin (Fd) is used as a scaffold for binding of a ruthenium photosensitizer and H-2 catalytic function is imparted to its partner protein, ferredoxin-NADP(+)-reductase (FNR), by attachment of cobaloxime molecules. We find that this 2-protein biohybrid system produces H-2 in aqueous solutions via light-induced interprotein electron transfer reactions (TON > 2500 H-2/FNR), providing insight about using native protein-protein interactions as a method for fuel generation.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1606243
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Photosynthesis Research
Additional Journal Information:
Journal Volume: 143; Journal Issue: 2
Country of Publication:
United States
Language:
English
Subject:
biohybrid; ferredoxin; ferredoxin-NADP+-reductase; photosynthetic electron transfer; solar fuel; solar hydrogen production

Citation Formats

Brahmachari, Udita, Pokkuluri, P. Raj, Tiede, David M., Niklas, Jens, Poluektov, Oleg G., Mulfort, Karen L., and Utschig, Lisa M. Interprotein electron transfer biohybrid system for photocatalytic H2 production. United States: N. p., 2020. Web. doi:10.1007/s11120-019-00705-x.
Brahmachari, Udita, Pokkuluri, P. Raj, Tiede, David M., Niklas, Jens, Poluektov, Oleg G., Mulfort, Karen L., & Utschig, Lisa M. Interprotein electron transfer biohybrid system for photocatalytic H2 production. United States. doi:10.1007/s11120-019-00705-x.
Brahmachari, Udita, Pokkuluri, P. Raj, Tiede, David M., Niklas, Jens, Poluektov, Oleg G., Mulfort, Karen L., and Utschig, Lisa M. Sat . "Interprotein electron transfer biohybrid system for photocatalytic H2 production". United States. doi:10.1007/s11120-019-00705-x.
@article{osti_1606243,
title = {Interprotein electron transfer biohybrid system for photocatalytic H2 production},
author = {Brahmachari, Udita and Pokkuluri, P. Raj and Tiede, David M. and Niklas, Jens and Poluektov, Oleg G. and Mulfort, Karen L. and Utschig, Lisa M.},
abstractNote = {Worldwide there is a large research investment in developing solar fuel systems as clean and sustainable sources of energy. The fundamental mechanisms of natural photosynthesis can provide a source of inspiration for these studies. Photosynthetic reaction center (RC) proteins capture and convert light energy into chemical energy that is ultimately used to drive oxygenic water-splitting and carbon fixation. For the light energy to be used, the RC communicates with other donor/acceptor components via a sophisticated electron transfer scheme that includes electron transfer reactions between soluble and membrane bound proteins. Herein, we reengineer an inherent interprotein electron transfer pathway in a natural photosynthetic system to make it photocatalytic for aqueous H-2 production. The native electron shuttle protein ferredoxin (Fd) is used as a scaffold for binding of a ruthenium photosensitizer and H-2 catalytic function is imparted to its partner protein, ferredoxin-NADP(+)-reductase (FNR), by attachment of cobaloxime molecules. We find that this 2-protein biohybrid system produces H-2 in aqueous solutions via light-induced interprotein electron transfer reactions (TON > 2500 H-2/FNR), providing insight about using native protein-protein interactions as a method for fuel generation.},
doi = {10.1007/s11120-019-00705-x},
journal = {Photosynthesis Research},
number = 2,
volume = 143,
place = {United States},
year = {2020},
month = {2}
}

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