An allosteric photoredox catalyst inspired by photosynthetic machinery

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

Research output: Contribution to journalArticle

30 Citations (Scopus)

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. Thus, 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.

Original languageEnglish
Article number6541
JournalNature Communications
Volume6
DOIs
Publication statusPublished - 2015

Fingerprint

machinery
Machinery
Light
catalysts
Catalysts
antennas
Antennas
Allosteric Regulation
Solar Energy
Optics and Photonics
Ligands
solar energy conversion
Photonic devices
ligands
Catalysis
Energy conversion
Solar energy
Oxidation-Reduction
catalysis
catalytic activity

ASJC Scopus subject areas

  • Biochemistry, Genetics and Molecular Biology(all)
  • Chemistry(all)
  • Physics and Astronomy(all)

Cite this

Lifschitz, A. M., Young, R. M., Mendez-Arroyo, J., Stern, C. L., McGuirk, C. M., Wasielewski, M. R., & Mirkin, C. A. (2015). An allosteric photoredox catalyst inspired by photosynthetic machinery. Nature Communications, 6, [6541]. https://doi.org/10.1038/ncomms7541

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.

In: Nature Communications, Vol. 6, 6541, 2015.

Research output: Contribution to journalArticle

Lifschitz, AM, Young, RM, Mendez-Arroyo, J, Stern, CL, McGuirk, CM, Wasielewski, MR & Mirkin, CA 2015, 'An allosteric photoredox catalyst inspired by photosynthetic machinery', Nature Communications, vol. 6, 6541. https://doi.org/10.1038/ncomms7541
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. In: Nature Communications. 2015 ; Vol. 6.
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