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Title: An allosteric photoredox catalyst inspired by photosynthetic machinery

Abstract

Biological photosynthetic machinery allosterically regulate light harvesting via conformational and electronic changes at the antenna protein complexes as a response to specific chemical inputs. Fundamental limitations in current approaches to regulating inorganic light-harvesting mimics prevent their use in catalysis. Here we show that a light-harvesting antenna/reaction centre mimic can be regulated by utilizing a coordination framework incorporating antenna hemilabile ligands and assembled via a high-yielding, modular approach. As in nature, allosteric regulation is afforded by coupling the conformational changes to the disruptions in the electrochemical landscape of the framework upon recognition of specific coordinating analytes. The hemilabile ligands enable switching using remarkably mild and redox-inactive inputs, allowing one to regulate the photoredox catalytic activity of the photosynthetic mimic reversibly and in situ. Furthermore, we demonstrate that bioinspired regulatory mechanisms can be applied to inorganic light-harvesting arrays displaying switchable catalytic properties and with potential uses in solar energy conversion and photonic devices.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1370514
Grant/Contract Number:  
SC0001059
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); bio-inspired; hydrogen and fuel cells; electrodes - solar; defects; charge transport; spin dynamics; membrane; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

Lifschitz, Alejo M., Young, Ryan M., Mendez-Arroyo, Jose, Stern, Charlotte L., McGuirk, C. Michael, Wasielewski, Michael R., and Mirkin, Chad A. An allosteric photoredox catalyst inspired by photosynthetic machinery. United States: N. p., 2015. Web. doi:10.1038/ncomms7541.
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Lifschitz, Alejo M., Young, Ryan M., Mendez-Arroyo, Jose, Stern, Charlotte L., McGuirk, C. Michael, Wasielewski, Michael R., & Mirkin, Chad A. An allosteric photoredox catalyst inspired by photosynthetic machinery. United States. https://doi.org/10.1038/ncomms7541
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Lifschitz, Alejo M., Young, Ryan M., Mendez-Arroyo, Jose, Stern, Charlotte L., McGuirk, C. Michael, Wasielewski, Michael R., and Mirkin, Chad A. Mon . "An allosteric photoredox catalyst inspired by photosynthetic machinery". United States. https://doi.org/10.1038/ncomms7541. https://www.osti.gov/servlets/purl/1370514.
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@article{osti_1370514,
title = {An allosteric photoredox catalyst inspired by photosynthetic machinery},
author = {Lifschitz, Alejo M. and Young, Ryan M. and Mendez-Arroyo, Jose and Stern, Charlotte L. and McGuirk, C. Michael and Wasielewski, Michael R. and Mirkin, Chad A.},
abstractNote = {Biological photosynthetic machinery allosterically regulate light harvesting via conformational and electronic changes at the antenna protein complexes as a response to specific chemical inputs. Fundamental limitations in current approaches to regulating inorganic light-harvesting mimics prevent their use in catalysis. Here we show that a light-harvesting antenna/reaction centre mimic can be regulated by utilizing a coordination framework incorporating antenna hemilabile ligands and assembled via a high-yielding, modular approach. As in nature, allosteric regulation is afforded by coupling the conformational changes to the disruptions in the electrochemical landscape of the framework upon recognition of specific coordinating analytes. The hemilabile ligands enable switching using remarkably mild and redox-inactive inputs, allowing one to regulate the photoredox catalytic activity of the photosynthetic mimic reversibly and in situ. Furthermore, we demonstrate that bioinspired regulatory mechanisms can be applied to inorganic light-harvesting arrays displaying switchable catalytic properties and with potential uses in solar energy conversion and photonic devices.},
doi = {10.1038/ncomms7541},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Mon Mar 30 00:00:00 EDT 2015},
month = {Mon Mar 30 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms7541
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Cited by: 47 works
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Figures / Tables:

Figure 1 Figure 1: Allosteric regulation of a light-harvesting antenna/reaction centre mimic. Activation of the catalytically active reaction centre mimic on the excitation of the antenna at 480 nm is controlled via coordination chemistry at a distal, redox-active Rh(I) centre. Light-harvesting antenna is shown in green and the reaction centre is shownmore » in magenta and blue.« less
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Crystal structure of spinach major light-harvesting complex at 2.72 Å resolution
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Molecular basis of photoprotection and control of photosynthetic light-harvesting
journal, July 2005

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Lessons from nature about solar light harvesting
journal, September 2011

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  • Nature Chemistry, Vol. 3, Issue 10
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Allosteric regulation and catalysis emerge via a common route
journal, July 2008

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Self-regulation of photoinduced electron transfer by a molecular nonlinear transducer
journal, May 2008

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Electronic energy harvesting multi BODIPY-zinc porphyrin dyads accommodating fullerene as photosynthetic composite of antenna-reaction center
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Architecture of a Charge-Transfer State Regulating Light Harvesting in a Plant Antenna Protein
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