An allosteric photoredox catalyst inspired by photosynthetic machinery

Lifschitz, Alejo M.; Young, Ryan M.; Mendez-Arroyo, Jose; Stern, Charlotte L.; McGuirk, C. Michael; Wasielewski, Michael R.; Mirkin, Chad A.

doi:10.1038/ncomms7541

An allosteric photoredox catalyst inspired by photosynthetic machinery

Journal Article · Mon Mar 30 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms7541· OSTI ID:1370514

Lifschitz, Alejo M. ^[1]; Young, Ryan M. ^[1]; Mendez-Arroyo, Jose ^[1]; Stern, Charlotte L. ^[1]; McGuirk, C. Michael ^[1]; Wasielewski, Michael R. ^[1]; Mirkin, Chad A. ^[1]

Northwestern Univ., Evanston, IL (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001059

OSTI ID:: 1370514

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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CCDC 1045099: Experimental Crystal Structure Determination: ZUCGAH : catena-[(μ-5,15-bis(4 (((2-(diphenylphosphino)ethyl)sulfanyl)methyl)phenyl)-10,20-dimesitylporphyrinato)-zinc unknown solvate] Space Group: C 2/c (15), Cell: a 28.4395(15)Å b 18.7648(11)Å c 16.3621(9)Å, α 90° β 123.051(3)° γ 90° Lifschitz, Alejo M.; Young, Ryan M.; Mendez-Arroyo, Jose https://doi.org/10.5517/cc142hwl The current record is supplemented by this dataset	dataset	January 2015
CCDC 1045100: Experimental Crystal Structure Determination: ZUCGEL : (N-(2-(diphenylphosphino)ethyl)(bis(4-ethyl-3,5-dimethyl-1H-pyrrol-2-yl))methaniminiumato)(difluoro)borate Space Group: P 21/c (14), Cell: a 8.4508(4)Å b 41.4961(16)Å c 8.0700(3)Å, α 90° β 94.122(4)° γ 90° Lifschitz, Alejo M.; Young, Ryan M.; Mendez-Arroyo, Jose https://doi.org/10.5517/cc142hxm The current record is supplemented by this dataset	dataset	January 2015
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An allosteric photoredox catalyst inspired by photosynthetic machinery

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