Jain Shailja, Danovich David, Shaik Sason
Institute of Chemistry, The Hebrew University of Jerusalem, Edmond J. Safra Campus, Givat Ram, Jerusalem 9190401, Israel.
J Phys Chem A. 2024 Jun 13;128(23):4595-4604. doi: 10.1021/acs.jpca.4c00437. Epub 2024 May 22.
This study uses computational means to explore the feasibility of N cleavage by frustrated Lewis pair (FLPs) species. The employed FLP systems are phosphane/borane () and carbene/borane (). Previous studies show that and react with H and CO but do not activate N. The present study demonstrates that N is indeed inert, and its activation requires augmentation of the FLPs by an external tool. As we demonstrate here, FLP-mediated N activation can be achieved by an external electric field oriented along the reaction axis of the FLP. Additionally, the study demonstrates that FLP -N activation generates useful nitrogen compound, e.g., hydrazine (HN-NH). In summary, we conclude that FLP effectively activates N in tandem with oriented external electric fields (OEEFs), which play a crucial role. This FLP/OEEF combination may serve as a general activator of inert molecules.
本研究采用计算手段探索受阻路易斯酸碱对（FLPs）物种对N进行裂解的可行性。所采用的FLP体系为膦/硼烷（）和卡宾/硼烷（）。先前的研究表明，和与H和CO反应，但不活化N。本研究表明，N确实是惰性的，其活化需要借助外部工具增强FLPs。正如我们在此所证明的，FLP介导的N活化可通过沿FLP反应轴定向的外部电场来实现。此外，该研究表明，FLP - N活化会生成有用的氮化合物，例如肼（HN - NH）。总之，我们得出结论，FLP与定向外部电场（OEEFs）协同作用可有效活化N，其中定向外部电场起着关键作用。这种FLP/OEEF组合可能用作惰性分子的通用活化剂。
