Consecutive ligand-based PCET processes affording a doubly reduced nickel pyrazinedithiolate which transforms into a metal hydride required to evolve H 2

Keita Koshiba, Kosei Yamauchi, Ken Sakai

Research output: Contribution to journalArticlepeer-review

15 Citations (Scopus)

Abstract

Our DFT results demonstrate that hydrogen evolution from water catalyzed by a nickel pyradinedithiolate (dcpdt) molecular hydrogen evolution catalyst [Ni II (dcpdt) 2 ] 2− proceeds via the formation of a square-planar nickel(ii) hydride intermediate which is given by unprecedented structural transformation of a doubly reduced triply protonated species [Ni II (dcpdtH 2 )(dcpdtH)] , afforded as a result of two consecutive ligand-based reductions of [Ni II (dcpdt)(dcpdtH)] through proton-coupled electron transfer (PCET) pathways.

Original languageEnglish
Pages (from-to)635-640
Number of pages6
JournalDalton Transactions
Volume48
Issue number2
DOIs
Publication statusPublished - 2019

All Science Journal Classification (ASJC) codes

  • Inorganic Chemistry

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