Journal
ACS NANO
Volume 15, Issue 5, Pages 8621-8637Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c00486
Keywords
pallidum nanoparticle; heterogeneous catalysis; Suzuki-Miyaura reaction; structure evolution; identical location transmission electron microscopy (IL-TEM)
Categories
Funding
- National Natural Science Foundation of China [21773269, 22072164, 21761132025, 51932005, 21703262]
- Liao Ning Revitalization Talents Program [XLYC1807175]
- Research Fund of SYNL
- Youth Innovation Promotion Association CAS [2015152]
Ask authors/readers for more resources
The mechanism of palladium nanoparticles-catalyzed cross-coupling reactions has been intensively debated due to the active sites involving dynamic changed Pd species. Through experimental methods, the study revealed that leached Pd components could significantly contribute to the coupling products, with different substrates showing varying degrees of influence. Additionally, the evolution of supported Pd NPs, including dissolution, deposition, and growth, was spatially and temporally observed, providing valuable insights for understanding the mechanism of heterogeneous Pd-catalyzed Suzuki coupling reactions.
The mechanism of palladium nanoparticles (PdNPs)-catalyzed cross-coupling reactions has been the subject of intense debate since the recognition of catalytic active sites involving a wide array of dynamic changed Pd species. Here, through the combination of the hot filtration experiment together with the recently developed identical location transmission electron microscopy (IL-TEM) method, the delicate structure evolution of highly dispersed Pd NPs supported on oxygen-functionalized carbon nanotubes (Pd/oCNTs) as well as the kinetics properties of derived dissolved species in liquid phase were systemically investigated in the Suzuki-Miyaura reaction. The result indicates that the leached Pd components caused by the strong adsorption of reactants might have a significant contribution to the coupling products, and the degree for different substrates follows the order of iodobenzene > phenylboronic acid > bromobenzene. Meanwhile, the typical three sequential behaviors of supported Pd NPs, including dissolution, deposition, and growth, along with the increase of the conversion throughout the reaction were spatiotemporally observed by tracking the evolution of individually identifiable NPs. The performed work not only provides direct evidence for the interaction between Pd NPs surface with reactants on atomic scale but also gives a valuable reference for fundamentally understanding the mechanism of the heterogeneous Pd-catalyzed Suzuki coupling process as well as rational design of next-generation catalysts with high efficiency and reusability for synthetic applications.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available