Krishnan Chandu G, Takano Hideaki, Katsuyama Hitomi, Kanna Wataru, Hayashi Hiroki, Mita Tsuyoshi
Institute for Chemical Reaction Design and Discovery (WPI-ICReDD), Hokkaido University, Kita 21, Nishi 10, Kita-ku, Sapporo, Hokkaido 001-0021, Japan.
JST, ERATO Maeda Artificial Intelligence in Chemical Reaction Design and Discovery Project, Kita 10, Nishi 8, Kita-ku, Sapporo, Hokkaido 060-0810, Japan.
JACS Au. 2024 Jul 29;4(10):3777-3787. doi: 10.1021/jacsau.4c00347. eCollection 2024 Oct 28.
Diphosphine ligands based on cyclobutane, bicyclo[3.1.1]heptane, and bicyclo[4.1.1]octane were synthesized from the corresponding highly strained, small, cyclic organic molecules, i.e., bicyclo[1.1.0]butane, [3.1.1]propellane, and [4.1.1]propellane, employing a ring-opening diphosphination. Under photocatalytic conditions, the three-component reaction of a diarylphosphine oxide, one of the aforementioned strained molecules, and a diarylchlorophosphine results in the smooth formation of the corresponding diphosphines in high yield. The obtained diphosphines can be expected to find applications in functional molecules due to their unique structural characteristics, which likely impart specific properties on their associated metal complexes and coordination polymers (e.g., a zigzag-type structure). The feasibility of the initial radical addition can be estimated using density-functional-theory calculations using the artificial force induced reaction (AFIR) method. This study focuses on the importance of integrating experimental and computational methods for the design and synthesis of new diphosphination reactions that involve strained, small, cyclic organic molecules.
基于环丁烷、双环[3.1.1]庚烷和双环[4.1.1]辛烷的二膦配体是由相应的高张力、小的环状有机分子,即双环[1.1.0]丁烷、[3.1.1]丙二烯和[4.1.1]丙二烯,通过开环二膦化反应合成的。在光催化条件下,二芳基氧化膦、上述张力分子之一与二芳基氯膦的三组分反应能顺利地高产率生成相应的二膦。由于所获得的二膦具有独特的结构特征,预计它们可在功能分子中得到应用,这些结构特征可能赋予其相关金属配合物和配位聚合物特定的性质(例如锯齿形结构)。初始自由基加成的可行性可以使用人工力诱导反应(AFIR)方法通过密度泛函理论计算来估计。本研究着重于整合实验和计算方法对于涉及高张力、小的环状有机分子的新型二膦化反应的设计和合成的重要性。