期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 28, 期 16, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202104339
关键词
Zeolites; NH4F etching; Dissolution mechanism; Mesopore; Diffusion
资金
- Thousand Talents Program for Foreign Experts [WQ20152100316]
- NSFC [21991090, NSFC21991091]
- Bulgarian Ministry of Education and Science [D01-76/2021]
- [NSFC22178389]
- [NSFC21975285]
The formation of mesopores in zeolite crystals is influenced by the zeolite architecture at both nano- and sub-nano scales. The dissolution behavior of zeolites is determined by the spatio-temporal dissolution of the framework at the nano-scale, and the diffusivity of reactants and dissolved products at the sub-nano scale. These findings have important implications for understanding zeolite dissolution behavior and designing hierarchical zeolites.
The mesopores formation in zeolite crystals has long been considered to occur through the stochastic hydrolysis and removal of framework atoms. Here, we investigate the NH4F etching of representative small, medium, and large pore zeolites and show that the zeolite dissolution behavior, therefore the mesopore formation probability, is dominated by zeolite architecture at both nano- and sub-nano scales. At the nano-scale, the hidden mosaics of zeolite structure predetermine the spatio-temporal dissolution of the framework, hence the size, shape, location, and orientation of the mesopores. At the sub-nano scale, the intrinsic micropore size and connectivity jointly determine the diffusivity of reactant and dissolved products. As a result, the dissolution propensity varies from removing small framework fragments to consuming nanodomains and up to full digestion of the outmost part of zeolite crystals. The new knowledge will lead to new understanding of zeolite dissolution behavior and new adapted strategies for tailoring hierarchical zeolites.
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