期刊
NANO RESEARCH
卷 12, 期 10, 页码 2589-2596出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-019-2491-8
关键词
water-soluble; Pd; nanoclusters; catalysis; p-nitrophenol
类别
资金
- National Natural Science Foundation of China [21722308, 21802146]
- Beijing Natural Science Foundation [2192064]
- CAS Key Research Project of Frontier Science [QYZDB-SSW-SLH024]
- Frontier Cross Project of National Laboratory for Molecular Sciences [051Z011BZ3]
Hydrogenation of p-nitrophenol (PNP) towards the conversion to p-aminophenol (PAP) by metal catalysis is known as a simple and eco-friendly technique for the production of corresponding industrial and pharmaceutical intermediates. While continuous efforts are paid for more sustainable and greener procedures by using transition metal catalysts, atomic-precise reaction mechanism for the PNP-to-PAP is still illusive to be fully understood. Utilizing a dry-wet combined strategy, here we have synthesized water-soluble Pd-8 nanoclusters (NCs) with mercaptosuccinic acid (H(2)SMA) as the ligand, and the Pd-8 NCs found high catalytic performance for the conversion of PNP-to-PAP, as identified by the electrospray ionization mass spectrometer (ESI-MS) measurement. The gradual changes over time of ultraviolet-visible (UV-vis) spectra of PNP really display the catalytic reduction by NaBH4 in presence of Pd-8 NCs. Further, in-depth charge transfer interactions between PNP and the Pd-8 clusters at the proton-rich conditions are investigated by natural bond orbital (NBO) analysis and electron density difference (EDD) analysis. The exothermic and kinetic-favorable reaction pathways are addressed, based on successive PNP hydrogenation and H2O removal processes, clarifying the reaction mechanism of Pd catalysts. It is worth noting that this solid-state synthetic route for such Pd-8 clusters enables gram-scale quantity of production in likely practical use.
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