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Oxygen Coordination Promotes Single-Atom Cu(II)-Catalyzed Azide–Alkyne Click Chemistry without Reducing Agents

Tingting Yu,Lei Tao,Zhiyi Liu,Xuge Zhang,Tao Gan,Wensheng Yan,Lirong Zheng,Ge Meng,Wei Chen,Shoujie Liu,Chenliang Ye,Jian Zhang

Unique active sites make single-atom (SA) catalysts promising to overcome obstacles in homogeneous catalysis but challenging due to their fixed coordination environment. Click chemistry is restricted by the low activity of more available Cu(II) catalysts without reducing agents. Herein, we develop efficient, O-coordinated SA Cu(II) directly catalyzed click chemistry. As revealed by theoretical calculations of the superior coordination structure to promote the click reaction, an organic molecule-assisted strategy is applied to prepare the corresponding SA Cu catalysts with respective O and N coordination. Although they both belong to Cu(II) centers, the O-coordinated one exhibits a 5-fold higher activity than the other and even much better activity than traditional homogeneous and heterogeneous Cu(II) catalysts. Control experiments further proved that the O-coordinated SA Cu(II) catalyst tends to be reduced by alkyne into Cu acetylide rather than the N-coordinated catalyst and thus facilitates click chemistry.