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通过氧化物支持的 - 复合物来减少和功能化二,以形成氨或酸衍生物

R A Keerthi Shivaraam¹, Thayalan Rajeshkumar², Rosario Scopelliti³

¹Group of Coordination Chemistry, Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.

Angewandte Chemie (International ed. in English)

|October 12, 2024

概括

含有二 (N2) 的兰化物复合物开发不足. 这项研究合成了激活N2的新型异金属Tm/K复合体,使其随后功能化为氨和氨衍生物.

科学领域:

有机金属化学有机金属化学
兰化物化学兰化物化学
固定的方法是固定.

背景情况:

化物 (N2) 化学在化物复合物中比在d块金属中更少被探索.
在精确定义的兰化物复合体内对N2的功能化仍然是一个重大挑战.
开发用于N2激活的新合成路径对于化学至关重要.

研究的目的:

合成和表征新型异金属胺-复合物.
研究这些新复合体中的二协调和反应性.
探索这些复合体在N2功能化反应中的潜力.

主要方法:

氧化物支持的异金属 (Tm) 和 (K) 复合物的合成.
使用SQUID磁力测量,电子磁共振 (EPR),密度函数理论 (DFT) 计算和X射线晶体学进行了表征.
研究与质子 (H+) 和甲基三酸盐 (MeOTf) 的反应性.

主要成果:

成功合成了两个异金属复合物,即[{KTm(OSi(O^tBu) 3) 3}2(μ-η2 : η2-N2) ] (1) 和[K3{Tm(OSi(O^tBu) 3) 3}2(μ-η2 : η2-N2) ] (2).
复合体2具有罕见的N2^3-基联体,由两个Tm和三个K稳定,促进N2功能化.
结合K3Tm2的N2^3-部分与H+反应产生NH4Cl (18%的产量),并与MeOTf反应形成二甲基化物复合物 (3),该复合物在质溶解时产生MeHN-NMeH·2HCl (18%的产量).

结论:

这项研究通过介绍新的TM/K复合体,扩大了化化学的范围.
复合体2中独特的结构图案使N2^3-连接体的功能化成为可能.
证明对质子化和化的反应性为N2减少和C-N键形成开辟了途径,使用兰化物系统.

关键词:

二化合物复合体是二化合物的复合体.兰他化物兰他化物的功能化.氧化物联结体氧化物联结体这里是thuliumum.

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