Consideration of the Aluminum Distribution in Zeolites in Theoretical and Experimental Catalysis Research
Consideration of the Aluminum Distribution in Zeolites in Theoretical and Experimental Catalysis Research
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DOI：
10.1021/acscatal.7b03676
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发表时间：
2018-02-01
期刊：
影响因子：
12.9
通讯作者：
Gounder, Rajamani
中科院分区：
文献类型：
--
作者：
Knott, Brandon C.;Nimlos, Claire T.;Gounder, Rajamani
沸石催化的研究工作已经越来越认识到由骨架铝原子分布引起的结构和功能的多样性，通过新兴的催化现象的报道，这些催化现象超出了那些可识别为其早期历史的形状选择性的象征。活性中心分布如何影响催化的分子水平的描述是在实验和理论研究中经常阐述的理想目标，但它们受到沸石材料的结构和行为的不精确知识的限制。在实验研究中，更高的精度可以从合成过程中更可靠的结构控制和更强大的和定量的结构和动力学表征探针。在理论研究中，构建具有特定铝位置和分布的模型很少捕获实验研究的材料固有的异质性。在这个角度来看，我们讨论的研究结果，适当的框架的挑战，在开发更预测的合成结构功能关系的沸石，突出的研究ZSM-5沸石是结构最复杂的分子筛框架和最广泛的研究，因为它们的多功能性在商业应用中。我们讨论了研究方向，以解决这些挑战，并建立更强的沸石结构，组成和活性位点之间的连接，催化功能。这种联系有望帮助弥合理论和实验催化研究的发现，并将沸石活性位点设计从经验奋进转变为基于验证模型的更可预测的科学。
Research efforts in zeolite catalysis have become increasingly cognizant of the diversity in structure and function resulting from the distribution of framework aluminum atoms, through emerging reports of catalytic phenomena that fall outside those recognizable as the shape-selective ones emblematic of its earlier history. Molecular-level descriptions of how active-site distributions affect catalysis are an aspirational goal articulated frequently in experimental and theoretical research, yet they are limited by imprecise knowledge of the structure and behavior of the zeolite materials under interrogation. In experimental research, higher precision can result from more reliable control of structure during synthesis and from more robust and quantitative structural and kinetic characterization probes. In theoretical research, construction of models with specific aluminum locations and distributions seldom capture the heterogeneity inherent to the materials studied by experiment. In this Perspective, we discuss research findings that appropriately frame the challenges in developing more predictive synthesis-structure-function relations for zeolites, highlighting studies on ZSM-5 zeolites that are among the most structurally complex molecular sieve frameworks and the most widely studied because of their versatility in commercial applications. We discuss research directions to address these challenges and forge stronger connections between zeolite structure, composition, and active sites to catalytic function. Such connections promise to aid in bridging the findings of theoretical and experimental catalysis research, and transforming zeolite active site design from an empirical endeavor into a more predictable science founded on validated models.