Frank Neese

Dec 13, 2024 | nature.com | Lukas Kaltschnee |Andrey N. Pravdivtsev |Manuel Gehl |Gangfeng Huang |Christoph Riplinger |Frank Neese | +7 more

Hydrogenases are widespread metalloenzymes used for the activation and production of molecular hydrogen. Understanding the catalytic mechanism of hydrogenases can help to establish industrial (bio)catalytic hydrogen production and conversion. Here we show the observation of so-far undetectable intermediates of [Fe]-hydrogenase in its catalytic cycle. We observed these intermediates by applying a signal-enhancing NMR technique based on parahydrogen. Molecular hydrogen occurs as orthohydrogen or parahydrogen, depending on its nuclear spin state. We found that catalytic conversion of parahydrogen by the [Fe]-hydrogenase leads to notably enhanced NMR signals (parahydrogen-induced polarization, PHIP). The observed signals encode information about how the [Fe]-hydrogenase binds hydrogen during catalysis. Our data support models of the catalytic mechanism that involve the formation of a hydride at the iron centre. Moreover, PHIP enabled studying the binding kinetics. This work demonstrates the hitherto unexploited power of PHIP to study catalytic mechanisms of hydrogenases. The catalytic mechanism of [Fe]-hydrogenases is not well understood. Now a signal-enhanced nuclear magnetic resonance method based on parahydrogen is introduced to study [Fe]-hydrogenase under turnover conditions in situ, revealing intermediates of the catalytic cycle.

Sep 9, 2024 | pubs.rsc.org | Michael Franz |Frank Neese |Sabine Richert

Elucidation of the exchange interaction in photoexcited three-spin systems − a second-order perturbational approach Photogenerated three-spin systems show great potential for applications in the field of molecular spintronics. In these systems, the exchange interaction in the electronically excited state dictates their magnetic properties.

Apr 4, 2024 | pubs.rsc.org | Frank Neese

Article type Paper Accepted 28 Mar 2024 First published 04 Apr 2024 This article is Open Access Faraday Discuss., 2024, Accepted Manuscript F. Neese, Faraday Discuss., 2024, Accepted Manuscript , DOI: 10.1039/D4FD00056K This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.