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分子聚合催化剂的单次转化揭示了时空分辨反应。

Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions.

机构信息

Department of Chemistry, University of California, Irvine, Irvine, CA, 92617, USA.

出版信息

Angew Chem Int Ed Engl. 2017 Oct 23;56(44):13772-13775. doi: 10.1002/anie.201708284. Epub 2017 Sep 25.

Abstract

Multiple active individual molecular ruthenium catalysts have been pinpointed within growing polynorbornene, thereby revealing information on the reaction dynamics and location that is unavailable through traditional ensemble experiments. This is the first single-turnover imaging of a molecular catalyst by fluorescence microscopy and allows detection of individual monomer reactions at an industrially important molecular ruthenium ring-opening metathesis polymerization (ROMP) catalyst under synthetically relevant conditions (e.g. unmodified industrial catalyst, ambient pressure, condensed phase, ca. 0.03 m monomer). These results further establish the key fundamentals of this imaging technique for characterizing the reactivity and location of active molecular catalysts even when they are the minor components.

摘要

已经在生长的聚降冰片烯中精确定位了多个活跃的单个分子钌催化剂,从而揭示了传统的整体实验无法获得的反应动力学和位置信息。这是首次通过荧光显微镜对单个分子催化剂进行单轮成像,并允许在工业上重要的分子开环复分解聚合(ROMP)催化剂下检测单个单体反应,反应条件为合成相关条件(例如,未经修饰的工业催化剂、常压、凝聚相、约 0.03 m 单体)。这些结果进一步确立了该成像技术的关键原理,即使当它们是少量成分时,也可以用于表征活性分子催化剂的反应性和位置。

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