期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 18, 页码 5000-5005出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201800672
关键词
CO2 activation; femtochemistry; photochemistry; time-resolved IR spectroscopy; transition-metal complexes
资金
- Deutsche Forschungsgemeinschaft through the Collaborative Research Center 813 Chemistry at Spin Centers
- Deutsche Forschungsgemeinschaft [VO 593/7-1]
The activation of carbon dioxide by transition metals is widely recognized as a key step for utilizing this greenhouse gas as a renewable feedstock for the sustainable production of fine chemicals. However, the dynamics of CO2 binding and unbinding to and from the ligand sphere of a metal have never been observed in the time domain. The ferrioxalate anion is used in aqueous solution as a unique model system for these dynamics and femtosecond UV-pump mid-infrared-probe spectroscopy is applied to explore its photoinduced primary processes in a time-resolved fashion. Following optical excitation, a neutral CO2 molecule is expelled from the complex within about 500 fs to generate a highly intriguing pentacoordinate ferrous dioxalate that carries a bent carbon dioxide radical anion ligand, that is, a reductively activated form of CO2, which is end-on-coordinated to the metal center by one of its two oxygen atoms.
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