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Catalytic Three‐Component Machinery: Control of Catalytic Activity by Machine Speed
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-12-07 , DOI: 10.1002/anie.201709644
Indrajit Paul 1 , Abir Goswami 1 , Nikita Mittal 1 , Michael Schmittel 1
Affiliation  

Three supramolecular slider‐on‐deck systems DS1DS3 were obtained as two‐component aggregates from the sliders S1S3 and deck D with its three zinc porphyrin (ZnPor) binding sites. The binding of the two‐footed slider to the deck varies with the donor qualities of and the steric hindrance at the pyridine/pyrimidine (pyr) feet, and was effected by two Npyr→ZnPor interactions. Accordingly, the sliders move over the three zinc porphyrins in the deck at different speeds, namely with 32.2, 220, and 440 kHz at room temperature. The addition of N‐methylpyrrolidine as an organocatalyst to DS1DS3 generates catalytic three‐component machineries. By using a conjugate addition as a probe reaction, we observed a correlation between the operating speed of the slider‐on‐deck systems and the yields of the catalytic reaction. As the thermodynamic binding of the slider decreases, both the frequency of the sliding motion and the yield of the catalytic reaction increase.

中文翻译:

催化三组分机械:通过机器速度控制催化活性

从滑块S1 - S3和甲板D及其三个锌卟啉(ZnPor)结合位点获得了三个超分子甲板上系统DS1 - DS3,作为两组分聚集体。两脚滑子与平台的结合随吡啶/嘧啶(pyr)脚的供体质量和空间位阻而变化,并且受两个N pyr →ZnPor相互作用的影响。因此,滑块以不同的速度,即在室温下以32.2、220和440 kHz的速度在甲板上的三种锌卟啉上移动。在DS1DS3中添加N-甲基吡咯烷作为有机催化剂产生催化三组分机械。通过使用共轭加成作为探针反应,我们观察到了甲板上滑模系统的运行速度与催化反应的产率之间的相关性。随着滑块的热力学结合减小,滑动的频率和催化反应的产率均增加。
更新日期:2017-12-07
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