Cation-exchanged zeolites for the selective oxidation of methane to methanol†,Catalysis Science & Technology

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Cation-exchanged zeolites for the selective oxidation of methane to methanol†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2017-10-19 00:00:00 , DOI: 10.1039/c7cy01229b
Ambarish R. Kulkarni _{1,

2,

3,

4,

5} , Zhi-Jian Zhao _{1,

2,

3,

4,

5} , Samira Siahrostami _{1,

2,

3,

4,

5} , Jens K. Nørskov _{1,

2,

3,

4,

5} , Felix Studt _{6,

7,

8,

9,

10}

Affiliation

Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. In this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metal cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C–H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C–H activation products. Finally, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.

中文翻译：

阳离子交换沸石，可将甲烷选择性氧化为甲醇†

受廉价天然气资源日益增加的推动，大量的实验和计算研究工作集中于确定将甲烷直接转化为甲醇的选择性催化剂。阳离子交换的沸石是一类有前途的催化剂，在过去的十年中，阳离子交换的沸石的受欢迎程度一直稳定增长。在本文中，我们首先从概念的角度介绍该领域，并重点介绍理论在发展对反应的分子水平的理解中的作用。接下来，通过执行和分析大型数据库的密度泛函理论（DFT）计算，以计算各种过渡金属阳离子，沸石拓扑结构和活性位点基序，就活性位点的稳定性而言，我们展示了甲烷活化过程的统一图景，C–H键活化和甲醇萃取。基于活性位点稳定性和反应性的权衡，我们提出了一个框架，用于识别这些系统中新的，有前途的活性位点基序。此外，我们显示出高的甲醇选择性归因于C–H活化产物的强结合性质。最后，利用从这些分析中获得的原子和机械洞察力，我们总结了提高阳离子交换沸石的性能以实现与工业相关的转化所面临的主要挑战和未来策略。我们显示出高的甲醇选择性归因于C–H活化产物的强结合性质。最后，利用从这些分析中获得的原子和机械洞察力，我们总结了提高阳离子交换沸石的性能以实现与工业相关的转化所面临的主要挑战和未来策略。我们显示出高的甲醇选择性归因于C–H活化产物的强结合性质。最后，利用从这些分析中获得的原子和机械洞察力，我们总结了提高阳离子交换沸石的性能以实现与工业相关的转化所面临的主要挑战和未来策略。

更新日期：2017-10-19

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