期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 115, 期 49, 页码 12395-12400出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1809342115
关键词
formic acid dehydrogenation; vibrational cross-angle method; intermediate molecular structure
资金
- National Natural Science Foundation of China (NSFC) [NSFC-21627805, 21673004, 21821004]
- NSF [CHE-1503865]
- Ministry of Science and Technology of the People's Republic of China [2017YFA0204702]
- King Abdullah University of Science and Technology
- Schlumberger future faculty award
The molecular structure of a catalytically active key intermediate is determined in solution by employing 2D IR spectroscopy measuring vibrational cross- angles. The formate intermediate (2) in the formic acid dehydrogenation reaction catalyzed by a phosphorus-nitrogen (PNP)-P-3-Ru catalyst is elucidated. Our spectroscopic studies show that the complex features a formate ion directly attached to the Ru center as a ligand, and a proton added to the imine arm of the dearomatized (PNP)-P-3* ligand. During the catalytic process, the imine arms are not only reversibly protonated and deprotonated, but also interacting with the protic substrate molecules, effectively serving as the local proton buffer to offer remarkable stability with a turnover number (TON) over one million.
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