The production of hydrocarbons for the synthesis of readily available energy and multifunctional materials is of great importance in modern society. Zeolites have proven to be a boon for the targeted regulation of specific hydrocarbon as shape-selective catalyst in converting carbon resources. Yet our mechanistic understanding and quantitative description of shape-selectivity of zeolite catalysis remains rather limited, which restricts the upgrade of zeolite catalysts. Herein, we proposed quantitative principle of shape-selectivity for zeolite catalysis using methanol-to-hydrocarbons (MTH) as model. Combining with molecular simulations and infrared imaging, we unveil the competition of thermodynamic stability, preferential diffusion and favored secondary reactions between different hydrocarbons within zeolite framework are the essence of zeolite shape-selective catalysis. Notably, we provide methodology to in silico search for the optimal combination of framework topology and acidity properties of zeolites with operating conditions that potentially outperform commercial MTH catalysts to achieve high selectivity of desired hydrocarbon products.

中文翻译：

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用于甲醇制烃沸石合理筛选的择形催化定量原理

生产用于合成现成能源和多功能材料的碳氢化合物在现代社会中非常重要。沸石已被证明是有针对性地调节特定碳氢化合物作为碳资源转化中的择形催化剂的福音。然而，我们对沸石催化的形状选择性的机理理解和定量描述仍然相当有限，这限制了沸石催化剂的升级。在此，我们提出了以甲醇制烃 (MTH) 为模型的沸石催化形状选择性的定量原理。结合分子模拟和红外成像，我们揭示了热力学稳定性的竞争，沸石骨架内不同烃类之间的优先扩散和有利的二次反应是沸石择形催化的本质。值得注意的是，我们提供了方法在计算机上寻找沸石骨架拓扑结构和酸度特性的最佳组合，以及可能优于商业 MTH 催化剂的操作条件，以实现所需碳氢化合物产品的高选择性。