An environmental-friendly NH-SAPO-34 catalyst, easily obtained via ion exchange, was prepared and tested for its catalytic ozonation activity in NO oxidation under O-deficient conditions. Characterization results revealed the successful loading of NH on the Brønsted acidity of SAPO-34 after NHNO ion exchange. Surprisingly, the NH-SAPO-34 zeolite exhibited superior performance in the catalytic ozonation of NO. Ab initio molecular dynamics simulations demonstrated that the facile binding of NO and O, along with rapid dissociation of the intermediate (NO dimer), contributed to the enhanced catalytic performance of NH-SAPO-34 compared to H-SAPO-34. Additionally, the impact of various ammonium salts on the catalytic activity was investigated, stating clearly the NH coordination in the eight-membered ring windows as the active site. Thus, this study deepens our understanding of the NO ozonation dynamics catalyzed by NH-SAPO-34 and provides a promising method for synthesizing catalysts without expensive transition metals.

中文翻译：

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揭示 NH4-SAPO-34 沸石上 NO 臭氧化的增强反应活性：从头算分子动力学与实验特性相结合


制备了一种环境友好型 NH-SAPO-34 催化剂，可通过离子交换轻松获得，并测试其在缺氧条件下氧化 NO 的催化臭氧化活性。表征结果表明，NH4NO 离子交换后，SAPO-34 的 Brønsted 酸度成功负载 NH。令人惊讶的是，NH-SAPO-34沸石在NO催化臭氧化中表现出优异的性能。从头算分子动力学模拟表明，与 H-SAPO-34 相比，NO 和 O 的轻松结合以及中间体（NO 二聚体）的快速解离有助于增强 NH-SAPO-34 的催化性能。此外，还研究了各种铵盐对催化活性的影响，清楚地表明八元环窗口中的NH配位作为活性位点。因此，这项研究加深了我们对 NH-SAPO-34 催化的 NO 臭氧化动力学的理解，并为合成不含昂贵过渡金属的催化剂提供了一种有前景的方法。