journal article·2024-04-11

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

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Abstract

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.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Click Chemistry and Applications · Advanced biosensing and bioanalysis techniques · Nanocluster Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, Zhejiang, China

Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Department of Chemistry, Tsinghua University, Beijing 100084, China

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China

National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230029, China

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

School of Materials Science and Engineering, Anhui University, Hefei 230601, China

Department of Power Engineering, North China Electric Power University, Baoding 071003, Hebei, China

Funding

Postdoctoral Research Foundation of China · National Postdoctoral Program for Innovative Talents · China National Funds for Distinguished Young Scientists

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