Closed Synthetic Cycle for Nickel‐Based Dihydrogen Formation

Author:

Hosseinmardi Soosan1ORCID,Scheurer Andreas1ORCID,Heinemann Frank W.1ORCID,Marigo Nicola2ORCID,Munz Dominik2ORCID,Meyer Karsten1ORCID

Affiliation:

1. Department of Chemistry and Pharmacy Inorganic Chemistry Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU) Egerlandstraße 1 91058 Erlangen Germany

2. Inorganic Chemistry Coordination Chemistry Saarland University Campus C4.1 66123 Saarbrücken Germany

Abstract

AbstractDihydrogen evolution was observed in a two‐step protonation reaction starting from a Ni0 precursor with a tripodal N‐heterocyclic carbene (NHC) ligand. Upon the first protonation, a NiII monohydride complex was formed, which was isolated and fully characterized. Subsequent protonation yields H2 via a transient intermediate (INT) and an isolable NiII acetonitrile complex. The latter can be reduced to regenerate its Ni0 precursor. The mechanism of H2 formation was investigated by using a deuterated acid and scrutinized by 1H NMR spectroscopy and gas chromatography. Remarkably, the second protonation forms a rare nickel dihydrogen complex, which was detected and identified in solution and characterized by 1H NMR spectroscopy. DFT‐based computational analyses were employed to propose a reaction profile and a molecular structure of the Ni−H2 complex. Thus, a dihydrogen‐evolving, closed‐synthetic cycle is reported with a rare Ni−H2 species as a key intermediate.

Funder

Deutsche Forschungsgemeinschaft

Bundesministerium für Bildung und Forschung

Friedrich-Alexander-Universität Erlangen-Nürnberg

Publisher

Wiley

Subject

General Chemistry,Catalysis,Organic Chemistry

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