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Highly efficient low-oxidation-potential electroche...
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Pd2+-Initiated Formic Acid Decomposition: Plausible Pathways for C-H Activation of Formate
| Journal | ChemPhysChem |
|---|---|
| Author | Won Jong Lee, Yeon Jin Hwang, Joohoon Kim, Hyangsoo Jeong, and Chang Won Yoon |
| Citation | ChemPhysChem 2019, 20, 1?11 |
| DOI | http://doi.org/10.1002/cphc.201801088 |
Formic acid (HCOOH, FA) has long been considered as a promising hydrogen-storage material due to its efficient hydrogen release under mild conditions. In this work, FA decomposes to generate CO2 and H2 selectively in the presence of aqueous Pd2+ complex solutions at 333 K. Pd(NO3)2 was the most effective in generating H2 among various Pd2+ complexes explored. Pd2+ complexes were in situ reduced to Pd0 species by the mixture of FA and sodium formate (SF) during the course of the reaction. Since C H activation reaction of Pd2+-bound formate is occurred for both Pd2+ reduction and H2/CO2 gas generation, FA decomposition pathways using several Pd2+ species were explored using density functional theory (DFT) calculations. Rotation of formate bound to Pd2+, β-hydride elimination, and subsequent CO2 and H2 elimination by formic acid were examined, providing different energies for rate determining step depending on the ligand electronics and geometries coordinated to the Pd2+ complexes. Finally, Pd2+ reduction toward Pd0 pathways were explored computationally either by generated H2 or reductive elimination of CO2 and H2 gas.
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