Hydroxy-bridged resting states of a [NiFe]-hydrogenase unraveled by cryogenic vibrational spectroscopy and DFT computations

• Published in: Chemical science (Cambridge) Vol. 12; no. 6; pp. 2189 - 2197
• Main Authors: Caserta, Giorgio, Pelmenschikov, Vladimir, Lorent, Christian, Tadjoung Waffo, Armel F, Katz, Sagie, Lauterbach, Lars, Schoknecht, Janna, Wang, Hongxin, Yoda, Yoshitaka, Tamasaku, Kenji, Kaupp, Martin, Hildebrandt, Peter, Lenz, Oliver, Cramer, Stephen P, Zebger, Ingo
• Format: Journal Article
• Language: English
• Published: England Royal Society of Chemistry 18.02.2021; The Royal Society of Chemistry
• Subjects: Archives & records; Band theory; Banded structure; Chemistry; Clusters; Density functional theory; Format; Hydrogenase; Infrared spectroscopy; Intermetallic compounds; Iron 57; Iron compounds; Low temperature; Molecular structure; Nickel compounds; Oxidation; Soil bacteria; Spectrum analysis

The catalytic mechanism of [NiFe]-hydrogenases is a subject of extensive research. Apart from at least four reaction intermediates of H 2 /H + cycling, there are also a number of resting states, which are formed under oxidizing conditions. Although not directly involved in the catalytic cycle, the k...