Structural analysis of transient reaction intermediate in formic acid dehydrogenation catalysis using two-dimensional IR spectroscopy

Yufan Zhang, Xin Chen, Bin Zheng, Xunmin Guo, Yupeng Pan, Hailong Chen, Huaifeng Li, Shixiong Min, Chao Guan, Kuo-Wei Huang, Junrong Zheng

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

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 PN3P-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 PN3P* 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.
Original languageEnglish (US)
Pages (from-to)12395-12400
Number of pages6
JournalProceedings of the National Academy of Sciences
Volume115
Issue number49
DOIs
StatePublished - Nov 19 2018

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