Improving
the stability of porous materials for practical applications
is highly challenging. Aluminosilicate zeolites are utilized for adsorptive
and catalytic applications, wherein they are sometimes exposed to
high-temperature steaming conditions (∼1000 °C). As the
degradation of high-silica zeolites originates from the defect sites
in their frameworks, feasible defect-healing methods are highly demanded.
Herein, we propose a method for healing defects to create extremely
stable high-silica zeolites. High-silica (SiO2/Al2O3 > 240) zeolites with *BEA-, MFI-, and MOR-type topologies
could be stabilized by significantly reducing the number of defect
sites via a liquid-mediated treatment without using additional silylating
agents. Upon exposure to extremely high temperature (900–1150
°C) steam, the stabilized zeolites retain their crystallinity
and micropore volume, whereas the parent commercial zeolites degrade
completely. The proposed self-defect-healing method provides new insights
into the migration of species through porous bodies and significantly
advances the practical applicability of zeolites in severe environments.
Characteristics of zeolite formation, such as being kinetically slow and thermodynamically metastable, are the main bottlenecks that obstruct a fast zeolite synthesis. We present an ultrafast route, the first of its kind, to synthesize high-silica zeolite SSZ-13 in 10 min, instead of the several days usually required. Fast heating in a tubular reactor helps avoid thermal lag, and the synergistic effect of addition of a SSZ-13 seed, choice of the proper aluminum source, and employment of high temperature prompted the crystallization. Thanks to the ultra-short period of synthesis, we established a continuous-flow preparation of SSZ-13. The fast-synthesized SSZ-13, after copper-ion exchange, exhibits outstanding performance in the ammonia selective catalytic reduction (NH3 -SCR) of nitrogen oxides (NOx ), showing it to be a superior catalyst for NOx removal. Our results indicate that the formation of high-silica zeolites can be extremely fast if bottlenecks are effectively widened.
Nepheline group materials obtained by a thermal treatment of K2CO3-supported nanosized sodalite are identified as cost-effective materials which show promising activity and durability toward diesel soot combustion.
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