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Activating catalysts with mechanical force

delete2009-04-06
delete561
PRE
AI
A
Alessio Piermattei *
S
S. Karthikeyan
R
Rint P. Sijbesma
DOI:10.1038/NCHEM.167delete
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摘要

摘要

En 中文
Homogeneously catalysed reactions can be 'switched on' by activating latent catalysts. Usually, activation is brought about by heat or an external chemical agent. However, activation of homogeneous catalysts with a mechanical trigger has not been demonstrated. Here, we introduce a general method to activate latent catalysts by mechanically breaking bonds between a metal and one of its ligands. We have found that silver(I) complexes of polymer-functionalized N-heterocyclic carbenes, which are latent organocatalysts, catalyse a transesterification reaction when exposed to ultrasound in solution. Furthermore, ultrasonic activation of a ruthenium biscarbene complex with appended polymer chains results in catalysis of olefin metathesis reactions. In each case, the catalytic activity results from ligand dissociation, brought about by transfer of mechanical forces from the polymeric substituents to the coordination bond. Mechanochemical catalyst activation has potential applications in transduction and amplification of mechanical signals, and mechanically initiated polymerizations hold promise as a novel repair mechanism in self-healing materials.
Keyword:
OLEFIN METATHESIS CATALYSTS
N-HETEROCYCLIC CARBENES
ULTRASONIC DEGRADATION
COORDINATION
POLYMERS
MECHANOCHEMISTRY
POLYMERIZATION
BEARING
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期刊

Nature Chemistry 封面图
Nature Chemistry
IF:
20.2
论文数:
4.4K
被引数:
4.8W

机构

E
Eindhoven University of Technology
学者数:
1.6W
论文数: 1.5W
被引数: 2.2W
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