AI Article Synopsis
- Encapsulating noble metal species in zeolites can improve the performance and efficiency of catalysts used in thermal and environmental reactions, particularly with Ru which is a cost-effective alternative.
- The study developed a method combining hydrothermal processes and stepwise calcination to stabilize Ru clusters within MFI-type zeolite, leveraging special sites for better integration.
- Results indicate that the unique environment created by the Ru clusters and MFI enhances catalytic activity for alkane oxidation even at low temperatures, while maintaining stability up to 1000°C, thus providing important insights for future catalyst design.
Article Abstract
Achieving active and stable heterogeneous catalysts by encapsulating noble metal species within zeolites is highly promising for high utilization and cost efficiency in thermal and environmental catalytic reactions. Ru, considered an economical noble metal alternative with comparable performance, faces great challenges within MFI-type microporous zeolites due to its high cohesive energy and mobility. Herein, an innovative strategy was explored that couples hydrothermal in situ ligand protection with stepwise calcination in a flowing atmosphere to embed ultrasmall Ru clusters anchored at K-healed silanol sites (≡Si-Ru-O-K complexes) within 10-membered ring sinusoidal channels of MFI. Comprehensive experiments and theoretical calculations unveiled that the interplay between confined Ru clusters and MFI induces local strain in MFI, creating a unique catalytic microenvironment around the Ru clusters. This synergy interaction enhances alkane deep oxidation as the confined Ru clusters and the MFI microenvironment collectively pre-activate CH and O, facilitate the cleavage of C-H and C-C bonds at low temperatures. Notably, the stable geometric and electronic properties of the confined Ru show exceptional thermal stability up to 1000 °C, rivaling fresh catalysts. These findings shed vital methodological and mechanistic insights for developing efficacious heterogeneous catalysts for thermal catalysis.
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| http://dx.doi.org/10.1002/anie.202417618 | DOI Listing |
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