The cleavage and functionalization of CÀH bonds is of fundamental interest for both academia and industry. Generally, the transformation relies on transition metals,[1] which are involved in four major approaches: 1) electrophilic activation of the CÀH bond by a high- valent transition metal; 2) oxidative addition to the CÀH bond by low-valent transition metals; 3) CÀH bond activation by σ-bond metathesis, and 4) insertion of a metal carbenoid/ ...