研究目的
Investigating the synthesis of benzonitrile via electrochemical reduction and photolytic splitting of dinitrogen, utilizing a rhenium(III) pincer platform for nitrogen fixation.
研究成果
A three-step cycle for the generation of benzamide/benzonitrile from N2 was established, demonstrating the potential of metal-ligand cooperativity and photo- and electrochemical approaches in nitrogen fixation. The study highlights the importance of tuning the thermochemistry of N2 splitting and the role of the pincer ligand as a 2e–/2H+ reservoir.
研究不足
The study is limited by the low quantum yield of photolytic N2-splitting and the need for strong electrophiles for N-transfer. The thermal stability of the N2-bridged complex also poses challenges for thermal splitting.
1：Experimental Design and Method Selection:
The study involves the synthesis of a dinuclear N2-bridged complex through reduction of a rhenium(III) pincer platform, followed by photochemical splitting into terminal nitride complexes triggered by visible light.
2：Sample Selection and Data Sources:
The rhenium(III) precursor [ReCl2(PNPtBu)] (1) and its derivatives were used as samples.
3：List of Experimental Equipment and Materials:
A Xe arc lamp (λ > 305 nm) for photolysis, cyclic voltammetry (CV) for electrochemical studies, and single-crystal X-ray diffraction for structural confirmation.
4：Experimental Procedures and Operational Workflow:
The process includes electrochemical reduction, photochemical N2-splitting, and thermal N-transfer with benzoyl chloride.
5：Data Analysis Methods:
Density functional theory (DFT) for computational studies and NMR spectroscopy for product characterization.
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