Iron and Copper Active Sites in Zeolites and Their Correlation to Metalloenzymes,Chemical Reviews

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Iron and Copper Active Sites in Zeolites and Their Correlation to Metalloenzymes
Chemical Reviews ( IF 51.4 ) Pub Date : 2017-12-19 00:00:00 , DOI: 10.1021/acs.chemrev.7b00344
Benjamin E. R. Snyder ₁ , Max L. Bols ₂ , Robert A. Schoonheydt ₂ , Bert F. Sels ₂ , Edward I. Solomon _{1,

3}

Affiliation

Metal-exchanged zeolites are a class of heterogeneous catalysts that perform important functions ranging from selective hydrocarbon oxidation to remediation of NO_x pollutants. Among these, copper and iron zeolites are remarkably reactive, hydroxylating methane and benzene selectively at low temperature to form methanol and phenol, respectively. In these systems, reactivity occurs at well-defined molecular transition metal active sites, and in this review we discuss recent advances in the spectroscopic characterization of these active sites and their reactive intermediates. Site-selective spectroscopy continues to play a key role, making it possible to focus on active sites that exist within a distribution of inactive spectator metal centers. The definition of the geometric and electronic structures of metallozeolites has advanced to the level of bioinorganic chemistry, enabling direct comparison of metallozeolite active sites to functionally analogous Fe and Cu sites in biology. We identify significant parallels and differences in the strategies used by each to achieve high reactivity, highlighting potentially interesting mechanisms to tune the performance of synthetic catalysts.

中文翻译：

沸石中的铁和铜活性位及其与金属酶的关系

金属交换的沸石是一类执行测距从选择性烃氧化为NO的修复重要功能的非均相催化剂的_X污染物。其中，铜和铁沸石具有显着的反应性，可在低温下选择性地羟化甲烷和苯，分别形成甲醇和苯酚。在这些系统中，反应性发生在明确定义的分子过渡金属活性位点上，在本综述中，我们讨论了这些活性位点及其反应性中间体的光谱表征方面的最新进展。现场选择光谱学继续发挥关键作用，使人们有可能将注意力集中在非活动观众金属中心分布内的活动地点。金属沸石的几何和电子结构的定义已发展到生物无机化学的水平，从而可以直接比较金属沸石的活性位点与生物学上功能相似的Fe和Cu位点。

更新日期：2017-12-19

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