Understanding the nature of active sites in metal-supported catalysts is of great importance towards establishing their structure-property relationships. The outstanding catalytic performance of metal-supported catalysts is frequently ascribed to the synergic effect of different active sites, which is however not well spectroscopically characterized. Herein, we report the direct detection of surface Zn species and H- Zn internuclear interaction between Zn ions and Brønsted acid sites on Zn-modified ZSM-5 zeolites by high-field solid-state NMR spectroscopy. The observed promotion of C-H bond activation of methane is rationalized by the enhanced Brønsted acidity generated by synergic effects arising from the spatial proximity/interaction between Zn ions and Brønsted acidic protons. The concentration of synergic active sites is determined by H- Zn double-resonance solid-state NMR spectroscopy.
Microcapsule-based self-healing polymer materials are highly desirable because they can heal large-volume cracks without changing the original chemical structures of polymers. However, they are limited by processing difficulties and inhomogeneous distributions of two components. Herein, we report a one-component photoresponsive self-healing polymer composite with photoabsorbing hybrid microcapsules (PAHM), which gives the microcapsules photoabsorbing properties by introducing nano-TiO2 particles as photoabsorbing and emulsified agents in the poly(urea-formaldehyde)/TiO2 hybrid shells. Upon mechanical damage and then exposure to light, the photoresponsive healing agents in the cracks will be solidified to allow for self-healing, while the healing agents in the unbroken PAHM will be protected and remain unreacted, which endows this photoresponsive microcapsule-based self-healing composite with self-healing properties like those found in the conventional two-component microcapsule-based systems. Given the universality of this hybrid polymerization method, incorporation of the photoabsorbing particles to conventional polymer shells may further broaden the scope of applications of these widely used materials.
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