Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 16, Issue 48, Pages 14433-14438Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201002292
Keywords
collision induced dissociation; heterogeneous catalysis; mass spectrometry; organometallic complex; reactive landing
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Funding
- Chemical Sciences Division, Office of Basic Energy Sciences of the U.S. Department of Energy (DOE)
- Pacific Northwest National Laboratory (PNNL)
- U.S. DOE of Biological and Environmental Research and located at PNNL
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Organometallic complexes immobilized on surfaces combine the high selectivity of homogeneous catalysts with the ease of separation of catalyst from products attainable with heterogeneous catalysts. Here we report a novel approach for the highly controlled preparation of surface organometallic catalysts by gas-phase ligand stripping combined with reactive landing of mass-selected ions onto self-assembled monolayer surfaces. Collision-induced dissociation is used to generate highly reactive undercoordinated metal complexes in the gas-phase for subsequent surface immobilization. Complexes with an open coordination sell around the metal center are demonstrated to show enhanced activity towards reactive landing in comparison to fully ligated species. In situ TOF-SIMS analysis indicates that the immobilized complexes exhibit behavior consistent with catalytic activity when exposed to gaseous reagents.
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