(363ae) Enhancing Diffusion and Catalyst Lifetime of Zeolites By Novel Secondary Growth and Post-Treatment Methods

Research Interests Zeolite Synthesis and Catalysis, Hydrocarbon conversion, Material Characterization

Reducing limitations for internal molecular diffusion in zeolites is critical to improving catalyst activity and stability for commercial applications such as hydrocarbon cracking and methanol-to-hydrocarbons (MTH) reactions. The intrinsic confined pore networks in zeolite structures give rise to well-defined shape-selectivity, which can result in highly selective products, but oftentimes at the expense of reduced activity and lifetime owing to the large crystal sizes of conventional zeolites that impose mass transport restrictions. For example, zeolites with one-dimensional pores are highly selective to propylene in naptha cracking, but they deactivate faster than 2D or 3D analogues due to limited diffusion leading to extensive coking and pore mouth blockage. Such limitations can be overcome via a facile post-synthesis treatment to produce fins, which are small protrusions on external surfaces of seed crystals. This secondary growth technique has been demonstrated for zeolites with 3D (MFI) and 2D (FER) pore networks wherein finned catalysts markedly outperform their parent seeds in MTH and butene isomerization reactions, respectively. Here, we will discuss how this approach can be used to design finned 1D zeolites, using MTT as a prototypical example. Our findings show that molecular diffusion in finned MTT zeolites is faster, resulting in reduced rates of coking and longer catalyst lifetime relative to the conventional counterparts. Zeolites are also known to be prone to intrinsic defects during synthesis. We also demonstrate post-synthesis treatment methods aimed to reduce defects in zeolites thereby improving their diffusion properties and catalytic performance (e.g. total turnovers and lifetime) beyond what can be achieved with conventional as-synthesized materials.