N-H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer.
N-H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer.
复制标题
DOI：
10.1021/jacs.8b12957
复制
发表时间：
2019-02
影响因子：
15
通讯作者：
Dian Wang;Florian Loose;P. Chirik;R. Knowles
中科院分区：
文献类型：
--
作者：
Dian Wang;Florian Loose;P. Chirik;R. Knowles
报道了一种将氮化锰还原成氨的方法，其中光驱动的质子耦合电子转移使得能够形成弱N-H键。光还原（saltBu）MnVN氨和Mn（II）的配合物已完成使用9，10-二氢吖啶和适当匹配的光氧化还原催化剂和弱布朗斯特酸的组合。有效键解离自由能在35和46千卡/摩尔之间的酸还原剂对表现出高效率。这种光驱动的方法可以为在环境条件下催化均相氨合成的新方法提供蓝图。
A method for the reduction of a manganese nitride to ammonia is reported, where light-driven proton-coupled electron transfer enables the formation of weak N-H bonds. Photoreduction of (saltBu)MnVN to ammonia and a Mn(II) complex has been accomplished using 9,10-dihydroacridine and a combination of an appropriately matched photoredox catalyst and weak Brønsted acid. Acid-reductant pairs with effective bond dissociation free energies between 35 and 46 kcal/mol exhibited high efficiencies. This light-driven method may provide a blueprint for new approaches to catalytic homogeneous ammonia synthesis under ambient conditions.