Hydride state accumulation in native [FeFe]-hydrogenase with the physiological reductant H2 supports its catalytic relevance

Chem Commun (Camb). 2022 Jun 23;58(51):7184-7187. doi: 10.1039/d2cc00671e.

Abstract

Small molecules in solution may interfere with mechanistic investigations, as they can affect the stability of catalytic states and produce off-cycle states that can be mistaken for catalytically relevant species. Here we show that the hydride state (Hhyd), a proposed central intermediate in the catalytic cycle of [FeFe]-hydrogenase, can be formed in wild-type [FeFe]-hydrogenases treated with H2 in absence of other, non-biological, reductants. Moreover, we reveal a new state with unclear role in catalysis induced by common low pH buffers.

MeSH terms

  • Catalysis
  • Hydrogen / chemistry
  • Hydrogenase* / chemistry
  • Iron-Sulfur Proteins* / chemistry
  • Reducing Agents

Substances

  • Iron-Sulfur Proteins
  • Reducing Agents
  • Hydrogen
  • Hydrogenase