Journal
NANOSCALE
Volume 14, Issue 30, Pages 10980-10991Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2nr02765h
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Funding
- National Natural Science Foundation of China (NSFC) [21601094, 21401139, 21271139]
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In this study, ultrafine Pd nanoparticles were prepared using a single-ion precursor on a MOF-808 carrier, and a Pd-nano@MOF-808-Pza catalyst for hydrogenation reactions was obtained. The Pd-nano@MOF-808-Pza showed excellent catalytic activity in various reactions and density functional theory calculations provided insights into the chelation mechanism of Pd2+ ions on MOF-808.
Ultrafine Pd nanoparticles are prepared using a single-ion precursor on a MOF-808 carrier. The ligand 2,3-pyrazinedicarboxylic acid (Pza) is dispersed in porous MOF-808 via grafting on formic acid sites, and thus Pd2+ ions are chelated by Pza to form a new single-ion precursor Pd@MOF-808-Pza. Then a Pd-nano@MOF-808-Pza catalyst is prepared by direct reduction of this precursor using NaBH4. Material characterization reveals the homogeneous dispersion of 3-6 nm Pd nanoparticles within the MOF-808 matrix. Pd-nano@MOF-808-Pza exhibits excellent catalytic activity in the hydrogenation of unsaturated nitrogen-containing compounds, and other typical reactions, such as the Knoevenagel condensation, Suzuki/Heck cross-coupling, and hydrogen tandem reactions. In addition, density functional theory (DFT) calculations are carried out to elucidate the chelation of Pd2+ ions by Pza on MOF-808 and propose mechanisms of hydrogenation reactions. This work provides an effective reduction catalyst, and more importantly, a single-ion chelation strategy for design and synthesis of metal supported catalysts.
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