A Pyrene-Triazacyclononane Anchor Affords High Operational Stability for CO2 RR by a CNT-Supported Histidine-Tagged CODH

Umberto Contaldo; Mathieu Curtil; Julien Pérard; Christine Cavazza; Alan Le Goff

doi:10.1002/anie.202117212

A Pyrene-Triazacyclononane Anchor Affords High Operational Stability for CO₂ RR by a CNT-Supported Histidine-Tagged CODH

Angew Chem Int Ed Engl. 2022 May 16;61(21):e202117212. doi: 10.1002/anie.202117212. Epub 2022 Mar 23.

Authors

Umberto Contaldo^{1

2}, Mathieu Curtil¹, Julien Pérard², Christine Cavazza², Alan Le Goff¹

Affiliations

¹ Univ. Grenoble Alpes, CNRS, DCM, 38000, Grenoble, France.
² Univ. Grenoble Alpes, CEA, CNRS, IRIG, CBM, 38000, Grenoble, France.

Abstract

An original 1-acetato-4-(1-pyrenyl)-1,4,7-triazacyclononane (AcPyTACN) was synthesized for the immobilization of a His-tagged recombinant CODH from Rhodospirillum rubrum (RrCODH) on carbon-nanotube electrodes. The strong binding of the enzyme at the Ni-AcPyTACN complex affords a high current density of 4.9 mA cm^-2 towards electroenzymatic CO₂ reduction and a high stability of more than 6×10⁶ TON when integrated on a gas-diffusion bioelectrode.

Keywords: Azamacrocycles; CO2 Reduction; Carbon Monoxide Dehydrogenase; Carbon Nanotubes; Pyrene.

Publication types

Research Support, Non-U.S. Gov't

MeSH terms

Aldehyde Oxidoreductases* / metabolism
Aza Compounds
Carbon Dioxide / metabolism
Carbon Monoxide / metabolism
Histidine
Multienzyme Complexes* / metabolism
Nickel / metabolism
Piperidines
Pyrenes

Substances

Aza Compounds
Multienzyme Complexes
Piperidines
Pyrenes
triazacyclononane
Carbon Dioxide
Histidine
Nickel
Carbon Monoxide
Aldehyde Oxidoreductases