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Issue 37, 2018
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A photoactive semisynthetic metalloenzyme exhibits complete selectivity for CO2 reduction in water

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Abstract

A series of artificial metalloenzymes containing a ruthenium chromophore and [NiII(cyclam)]2+, both incorporated site-selectively, have been constructed within an azurin protein scaffold. These light-driven, semisynthetic enzymes do not evolve hydrogen, thus displaying complete selectivity for CO2 reduction to CO. Electrostatic effects rather than direct excited-state electron transfer dominate the ruthenium photophysics, suggesting that intramolecular electron transfer from photogenerated RuI to [NiII(cyclam)]2+ represents the first step in catalysis. Stern–Volmer analyses rationalize the observation that ascorbate is the only sacrificial electron donor that supports turnover. Collectively, these results highlight the important interplay of elements that must be considered when developing and characterizing molecular catalysts.

Graphical abstract: A photoactive semisynthetic metalloenzyme exhibits complete selectivity for CO2 reduction in water

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Supplementary files

Article information


Submitted
13 Feb 2018
Accepted
10 Apr 2018
First published
10 Apr 2018

Chem. Commun., 2018,54, 4681-4684
Article type
Communication
Author version available

A photoactive semisynthetic metalloenzyme exhibits complete selectivity for CO2 reduction in water

C. R. Schneider, A. C. Manesis, M. J. Stevenson and H. S. Shafaat, Chem. Commun., 2018, 54, 4681
DOI: 10.1039/C8CC01297K

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