[NiFe]-hydrogenases catalyze the reversible reaction H ⇄ 2H + 2e. Their basic module consists of a large subunit, coordinating the NiFe(CO)(CN) center, and a small subunit that carries electron-transferring iron-sulfur clusters. Here, we report the assembly of fully functional [NiFe]-hydrogenase starting from the isolated large and small subunits. Activity assays complemented by spectroscopic measurements revealed a native-like hydrogenase. This approach was used to label exclusively the NiFe(CO)(CN) center with Fe, enabling a clear view of the catalytic site by means of nuclear resonance vibrational spectroscopy. This strategy paves the way for in-depth studies of [NiFe]-hydrogenase catalytic intermediates.
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| http://dx.doi.org/10.1021/acscatal.0c04079 | DOI Listing |
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