The rational design of zeolite-based catalysts calls for flexible tailoring of porosity and acidity beyond micropore dimension. To date, dealumination has been applied extensively as an industrial technology for the tailoring of zeolite in micropore dimension, whereas desilication has separately shown its potentials in the creation of mesoporosities. The free coupling of dealumination with desilication will bridge the tailoring at micro/mesopore dimensions; however, such coupling has been prevailingly confirmed as an impossible mission. In this work, a consecutive dealumination-desilication process enables the introduction of uniform intracrystalline mesopores (4-6 nm) into the microporous Al-rich zeolites. The decisive impacts of steaming step have been firstly discovered. These findings revitalize the functions of dealumination in porosity tailoring, and stimulate the pursuit of new methods for the tailoring of industrially relevant Al-rich zeolites.

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It is extremely challenging to controllably synthesize rare earth‐containing nanoalloys due to the ultralow standard reduction potential of rare earth metals. Here, a surface‐confined strategy to prepare ultrafine Pt‐rare earth nanoalloys on a series of N‐functionalized supports is reported. It proves that by surface N‐metal coordination, the metal cations of precursors are atomically dispersed on support, which greatly favors uniform nucleation and growth of particles upon reduction. Moreover, the moderate metal transfer barrier from N ensures particle growth in a confined region to form ultrafine nanoalloys. Using this method, ultrafine PtLa, PtY, and PtDy nanoalloys are prepared on N‐functionalized supports such as carbon, zeolite, and Al2O3. Notably, the PtLa nanoalloys on N‐functionalized zeolite show superior activity and durability for propane oxidation. The strategy is expected to provide guidelines for preparing highly efficient rare earth‐containing nanoalloys for catalysis applications.