As a size- and shape-selective catalyst, zeolites are widely used in petroleum and fine-chemicals processing. However, their small micropores severely hinder molecular diffusion and are sensitive to coke formation. Hierarchically porous zeolite single crystals with fully interconnected, ordered, and tunable multimodal porosity at macro-, meso-, and microlength scale, like in leaves, offer the ideal solution. However, their synthesis remains highly challenging. Here, we report a versatile confined zeolite crystallization process to achieve these superior properties. Such zeolite single crystals lead to significantly improved mass transport properties by shortening the diffusion length while maintaining shape-selective properties, endowing them with a high efficiency of zeolite crystals, enhanced catalytic activities and lifetime, highly reduced coke formation, and reduced deactivation rate in bulky-molecule reactions and methanol-to-olefins process. Their industrial utilization can lead to the design of innovative and intensified reactors and processes with highly enhanced efficiency and minimum energy consumption.

作为尺寸和形状选择催化剂，沸石被广泛用于石油和精细化工加工中。然而，它们的小微孔严重阻碍了分子扩散并且对焦炭形成敏感。具有分层结构的多孔沸石单晶体具有完全互连的，有序的和可调的多尺度孔隙度（宏观，中观和微观长度尺度，如叶子），是理想的解决方案。然而，它们的合成仍然极具挑战性。在这里，我们报告了一种通用的受限沸石结晶过程，以实现这些优异的性能。此类沸石单晶可通过缩短扩散长度，同时保持形状选择特性，赋予沸石高效结晶性，增强催化活性和使用寿命，从而显着改善传质。大大减少了焦炭的形成，并降低了大分子反应和甲醇制烯烃工艺中的失活速率。它们在工业上的利用可以导致设计出具有高度提高的效率和最低能耗的创新型和强化型反应器和工艺。