Determination of the active form of the tetranuclear copper sulfur cluster in nitrous oxide reductase

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Abstract

N2OR has been found to have two structural forms of its tetranuclear copper active site, the 4CuS Cu-Z* form and the 4Cu2S Cu-Z form. EPR, resonance Raman, and MCD spectroscopies have been used to determine the redox states of these sites under different reductant conditions, showing that the Cu-Z* site accesses the 1-hole and fully reduced redox states, while the Cu-Z site accesses the 2-hole and 1-hole redox states. Single-turnover reactions of N2OR for Cu-Z and Cu-Z* poised in these redox states and steady-state turnover assays with different proportions of Cu-Z and Cu-Z* show that only fully reduced Cu-Z* is catalytically competent in rapid turnover with N2O.
Original languageEnglish
Pages (from-to)614-617
JournalJournal of the American Chemical Society
Volume136
Issue number2
DOIs
Publication statusPublished - 15 Jan 2014

Keywords

  • CU-Z CLUSTER
  • ACHROMOBACTER-CYCLOCLASTES
  • PSEUDOMONAS-NAUTICA
  • CATALYTIC CENTER
  • N2O REDUCTION
  • PURIFICATION
  • ENZYME
  • RESONANCE
  • MECHANISM
  • INSIGHT

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