Electrochemical Dinitrogen Splitting and Nitride Transfer to Nitric Oxide with Rhenium Pincer Complexes

by Lukas Alig
Doctoral thesis
Date of Examination:2022-03-24
Date of issue:2022-04-26
Advisor:Prof. Dr. Sven Schneider
Referee:Prof. Dr. Sven Schneider
Referee:Prof. Dr. Franc Meyer
Persistent Address: http://dx.doi.org/10.53846/goediss-9198

 

 

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Abstract

English

The Haber-Bosch process for the synthesis of ammonia from nitrogen and hydrogen consumes large amounts of energy and additionally relies on fossil feedstocks for the production of hydrogen. Alternative approaches for the synthesis of nitrogenous chemicals and in particular nitrogen oxides as part of fertilizer are therefore highly desirable. In this thesis, the formation of nitrous oxide is reported upon initial (electro)chemical dinitrogen splitting into nucleophilic Rhenium nitride complexes and subsequent nitride-NO coupling. The overall comproportionation of N2 and NO to N2O is investigated with spectroscopic methods and theoretical calculations and revealed a formal "umpolung" of the Rhenium nitride complex upon initial NO coordination.
Keywords: dinitrogen; N2 fixation; small molecule activation; N-N bond formation; Nitride Complex; Electrochemical N2 Splitting; DFT calculation; nitric oxide; nitrous oxide
 
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