N-doped carbon black (NCB) supported Ni NPs exhibited higher activity than most Ni-based catalysts for selective HDO of vanillin at mild conditions, ascribing to higher reducibility, lower oxidation state of Ni NPs and enhanced spillover hydrogen of Ni to NCB.
Processability of vitrimers strongly relies on the temperature dependence of viscosity. In this study, we analyzed temperature-dependent viscoelasticity of vitrimers based on the dioxaborolane metathesis reaction. A sol-to-gel transition process and a reverse gel-to-sol process are observed in the linear viscoelasticity with increasing content of the cross-linker. The latter gel-to-sol process is owing to a reverse reaction between a two-site interchain cross-linking point with an excess cross-linker, forming two noncross-linking sites. For samples above the gel point, the increasing temperature leads to a weaker acceleration of the decross-linking process than the Rouse-type relaxation, and accordingly, broadening of the plateau region. This trend is easily visualized in samples slightly above the gel point for which the stress relaxation arising from the Rouse-type relaxation and the decross-linking process are not well separated over time. This temperature-dependent behavior reflects a case that the lifetime of the dynamic covalent bond is significantly larger than the Rouse time of the network strands. As a result, the stress borne by a strand relaxes immediately upon decrosslinking, and thus, the low activation energy of the dioxaborolane metathesis reaction governs the strand relaxation.
Identification of the active copper species, and further illustration of the catalytic mechanism of Cu-based catalysts is still a challenge because of the mobility and evolution of Cu and Cu species in the reaction process. Thus, an unprecedentedly stable Cu-based catalyst was prepared by uniformly embedding Cu nanoparticles in a mesoporous silica shell allowing clarification of the catalytic roles of Cu and Cu in the dehydrogenation of methanol to methyl formate by combining isotope-labeling experiment, in situ spectroscopy, and DFT calculations. It is shown that Cu sites promote the cleavage of the O-H bond in methanol and of the C-H bond in the reaction intermediates CH O and H COOCH which is formed from CH O and HCHO, whereas Cu sites cause rapid decomposition of formaldehyde generated on the Cu sites into CO and H .
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