期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 48, 页码 16760-16763出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja5097489
关键词
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资金
- 973 Program from the MOST of China [2012CB725302]
- National Natural Science Foundation of China [21390400, 21025206, 21272180, 21302148, 21372266]
- Research Fund for the Doctoral Program of Higher Education of China [20120141130002]
- Program for Changjiang Scholars and Innovative Research Team in University [IRT1030]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Department of Energy
- Chemical Sciences, Geosciences and Bioscience Division, U.S. Department of Energy [DE-AC0-06CH11357]
- Chemical Sciences and Engineering Division at Argonne National Laboratory
An efficient alkyne C-H activation and homocoupling procedure has been studied which indicates that a Cu(II)/Cu(I) synergistic cooperation might be involved. In situ Raman spectroscopy was employed to study kinetic behavior, drawing the conclusion that Cu(I) rather than Cu(II) participates in the rate-determining step. IR, EPR, and X-ray absorption spectroscopy evidence were provided for structural information, indicating that Cu(I) has a stronger interaction with alkyne than Cu(II) in the C-H activation step. Kinetics study showed Cu(II) plays a role as oxidant in C-C bond construction step, which was a fast step in the reaction. X-band EPR spectroscopy showed that the coordination environment of CuCl2(TMEDA) was affected by Cu(I). A putative mechanism with Cu(I)-Cu(II) synergistic cooperation procedure is proposed for the reaction.
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