期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 49, 页码 19203-19207出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b09620
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis program [DE-SC0018977]
- Welch Foundation [A-1907]
The porosity and synthetic tunability of metal-organic frameworks (MOFs) has motivated interest in application of these materials as designer heterogeneous catalysts. While understanding substrate mobility in these materials is critical to the rational development of highly active catalyst platforms, experimental data are rarely available. Here we demonstrate kinetic isotope effect (KIE) analysis enables direct evaluation of the extent of substrate confinement as a function of material mesoporosity. Further, we provide evidence that suggests substrate confinement within a microporous Ru-2-based MOF gives rise to quantum tunneling during interstitial C-H amination. The reported data provide the first evidence for tunneling during interstitial MOF chemistry and illustrate an experimental strategy to evaluate the impact of material structure on substrate mobility in porous catalysts.
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