Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

Jessica F. Sonnenberg; Robert H. Morris

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Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

机译：区分均质与纳米颗粒不对称铁催化

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摘要

This perspective will examine the use of a wide range of techniques for differentiating homogeneous from nanoparticle asymmetric catalysis as it pertains to two highly active systems developed within our group. The 6,5,6 and 5,5,5-precatalysts, trans-[Fe(NCMe)CO(PPh2C6H4CH=NCHPh-)2][BF4]2 and trans-[Fe(CO)Br(PR2CH2CH=NCHPh-)2l[BF4], respectively, are highly active and selective asymmetric transfer hydrogenation (ATH) catalysts. Here, we will review the series of tests that were undertaken to support the idea that the 6,5,6-precatalyst forms iron nanoparticles (Fe NPs) during catalysis, whereas the 5,5,5-system remains homogeneous. Techniques include the use of NMR and DFT to investigate intermediates and activation steps, reaction profile and induction period analysis, substoichiometric poisoning, electron microscopy imaging, dynamic light scattering (DLS), X-ray photoelectron microscopy (XPS), magnetometry, and multiphasic analysis. We also elaborate on the wider applicability of these and other tests to probe the true nature of an active catalyst, with emphasis on the importance of using a wide range of techniques for insightful mechanistic evaluations.

机译：该观点将研究多种技术将均匀性与纳米颗粒不对称催化区分开，因为它与我们组中开发的两个高度活性系统有关。 6,5,6和5,5,5-催化剂，trans- [fe（ncme）co（pph2c6h4ch = nchph-）2] [bf4] 2和trans- [fe（co）br（pr2ch2ch = nchph-） 2L [BF4]分别是高度活性和选择性的不对称转移氢化（ATH）催化剂。在这里，我们将回顾一下为支持6,5,6-催化剂在催化过程中形成铁纳米颗粒（FE NP）的一系列测试，而5,5,5型系统保持均匀。技术包括使用NMR和DFT来研究中间体和激活步骤，反应曲线和诱导期分析，化学中毒，电子显微镜成像，动态光散射（DLS），X射线光电显微镜显微镜（XPS），磁力测定法和多性分析分析。我们还详细阐述了这些和其他测试的更广泛适用性，以探测活性催化剂的真实性质，重点是使用广泛的技术进行洞察力评估的重要性。

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来源
《Catalysis science & technology》 |2014年第10期|3426-3438|共13页
作者
Jessica F. Sonnenberg; Robert H. Morris;
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作者单位

Department ofChemistry, University of Toronto, 80 St. George Street, Toronto, Ontario, M5S 3H6, Canada.;

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原文格式 PDF
正文语种英语
中图分类汉语教学;
关键词
Iron; Catalysis; Nanoparticlesactive systemphotoelectron microscopywide-range;

机译：铁;催化;纳米粒子性系统photoelectron显微镜范围;

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Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

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