Activation of Ammonia by a Carbene-Stabilized Dithiolene Zwitterion
Activation of Ammonia by a Carbene-Stabilized Dithiolene Zwitterion
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卡宾稳定的二硫醇两性离子对氨的活化
DOI：
10.1021/jacs.2c07920
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发表时间：
2022
影响因子：
15
通讯作者：
Schaefer, Henry F.
中科院分区：
文献类型：
--
作者：
Wang, Yuzhong;Tran, Phuong M.;Lahm, Mitchell E.;Xie, Yaoming;Wei, Pingrong;Adams, Earle R.;Glushka, John N.;Ren, Zichun;Popik, Vladimir V.;Schaefer, Henry F.
卡宾稳定的二硫杂环戊二烯离子(3)通过单电子转移(SET)和氢原子转移(HAT)激活氨气，生成4·和5。用光谱分析和单晶X射线衍射法对反应产物进行了表征。用实验和计算的方法探讨了4·和5的形成机理。这一发现是通过HAT进行无金属氨活化的第一个例子。
A carbene-stabilized dithiolene zwitterion (3) activates ammonia, affording4•and5, through both single-electron transfer (SET) and hydrogen atom transfer (HAT). Reaction products were characterized spectroscopically and by single-crystal X-ray diffraction. The mechanism of the formation of4•and5was probed by experimental and computational methods. This discovery is the first example of metal-free ammonia activation via HAT.