期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 30, 页码 8680-8685出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201602930
关键词
dinuclear zinc complexes; homogeneous catalysis; metal-metal cooperativity; ring-opening polymerization; structure-activity relationship
资金
- EPSRC [EP/K035274/1, EP/K014070/1, EP/K014668/1, EP/L017393/1]
- Climate KIC
- University of Otago
- MacDiarmid Institute for Advanced Materials and Nanotechnology
- Engineering and Physical Sciences Research Council [EP/K014668/1, EP/K035274/1, EP/K014676/1, EP/L017393/1, EP/C544846/1, EP/C544838/1] Funding Source: researchfish
- EPSRC [EP/K014668/1, EP/K035274/1, EP/K014676/1, EP/L017393/1] Funding Source: UKRI
Understanding how to moderate and improve catalytic activity is critical to improving degradable polymer production. Here, di- and monozinc catalysts, coordinated by bis(imino)diphenylamido ligands, show remarkable activities and allow determination of the factors controlling performance. In most cases, the dizinc catalysts significantly outperform the monozinc analogs. Further, for the best dizinc catalyst, the ligand conformation controls activity: the catalyst with folded ligand conformation shows turnover frequency (TOF) values up to 60 000 h(-1) (0.1 mol% loading, 298 K, [LA]=1M), whilst that with a planar conformation is much slower, under similar conditions (TOF=30 h(-1)). Dizinc catalysts also perform very well under immortal conditions, showing improved control, and are able to tolerate loadings as low as 0.002 mol% whilst conserving high activity (TOF= 12500 h(-1)).
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