Pei Runbo, Chang Wenju, He Liancheng, Wang Tao, Zhao Yue, Liang Yong, Wang Xinping
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.
State Key laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai, China.
Nat Commun. 2024 Sep 11;15(1):7943. doi: 10.1038/s41467-024-52185-w.
Most C-H bond activations of natural gas alkanes rely on transition metal complexes. Activations by using main-group systems have been reported but required heating or photo-irradiation under high atmospheric pressure with rather low regioselectivity. Here we report that Lewis acid-carbene adducts facilely undergo oxidative additions to C-H bonds of ethane, propane and n-butane with high selectivity under room temperature and atmospheric pressure. The Lewis acids can be moved by the addition of a base and the carbene-derived products can be easily converted into aldehydes. This work offers a route for main-group element compounds to selectively functionalise C-H bonds of natural gas alkanes and other small molecules.
大多数天然气烷烃的C-H键活化依赖于过渡金属配合物。虽然已有使用主族体系进行活化的报道，但需要在高气压下加热或光照射，且区域选择性相当低。在此，我们报道路易斯酸-卡宾加合物在室温和大气压下能以高选择性轻松地对乙烷、丙烷和正丁烷的C-H键进行氧化加成。通过添加碱可以除去路易斯酸，并且卡宾衍生的产物可以很容易地转化为醛。这项工作为主族元素化合物选择性地官能团化天然气烷烃及其他小分子的C-H键提供了一条途径。
