Journal Article

PUBDB-2023-00996

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Stepwise assembly of the active site of [NiFe]-hydrogenase

Caserta, G. (Corresponding author) ; Hartmann, S. ; Van Stappen, C. ; Karafoulidi-Retsou, C. ; Lorent, C. ; Yelin, S. ; Keck, M. ; Schoknecht, J. ; Sergueev, I.XFEL.EU*DESY* ; Yoda, Y. ; Hildebrandt, P. ; Limberg, C. ; DeBeer, S. ; Zebger, I. ; Frielingsdorf, S. (Corresponding author) ; Lenz, O. (Corresponding author)

2023
Nature Publishing Group Basingstoke

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Please use a persistent id in citations: doi:10.1038/s41589-022-01226-w  doi:10.3204/PUBDB-2023-00996

Abstract: [NiFe]-hydrogenases are biotechnologically relevant enzymes catalyzing the reversible splitting of H$_2$ into 2e$^−$ and 2H$^+$ under ambient conditions. Catalysis takes place at the heterobimetallic NiFe(CN)$_2$(CO) center, whose multistep biosynthesis involves careful handling of two transition metals as well as potentially harmful CO and CN$^−$ molecules. Here, we investigated the sequential assembly of the [NiFe] cofactor, previously based on primarily indirect evidence, using four different purified maturation intermediates of the catalytic subunit, HoxG, of the O$_2$-tolerant membrane-bound hydrogenase from Cupriavidus necator. These included the cofactor-free apo-HoxG, a nickel-free version carrying only the Fe(CN)$_2$(CO) fragment, a precursor that contained all cofactor components but remained redox inactive and the fully mature HoxG. Through biochemical analyses combined with comprehensive spectroscopic investigation using infrared, electronic paramagnetic resonance, Mössbauer, X-ray absorption and nuclear resonance vibrational spectroscopies, we obtained detailed insight into the sophisticated maturation process of [NiFe]-hydrogenase.

Note: Funding:Einstein Foundation Berlin: grant number EVF-2016-277;SPP 1927 “Iron Sulfur for Life”: grants: DE1877/1-1 and 311062227;Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. Experimentebetreuung PETRA III (FS-PET-S)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
3. FS-Proposal: I-20200452 (I-20200452) (I-20200452)
4. DFG project 390540038 - EXC 2008: Unifying Systems in Catalysis "UniSysCat" (390540038) (390540038)

Experiment(s):

1. PETRA Beamline P01 (PETRA III)

Appears in the scientific report 2023

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Database coverage:
; ; BIOSIS Previews ; Biological Abstracts ; Clarivate Analytics Master Journal List ; Current Contents - Life Sciences ; DEAL Nature ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 10 ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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