Mechanistic Insight into Synergistic Catalysis of Olefin Hydrogenation by a Hetero-Dinuclear RuII–CoII Complex with Adjacent Reaction Sites
- Dachao Hong*Dachao Hong*E-mail: [email protected] (D.H.).Interdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, JapanMore by Dachao Hong,
- Yuji OhgomoriYuji OhgomoriInterdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, JapanMore by Yuji Ohgomori,
- Yoshihiro ShimoyamaYoshihiro ShimoyamaInterdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, JapanMore by Yoshihiro Shimoyama,
- Hiroaki KotaniHiroaki KotaniDepartment of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, JapanMore by Hiroaki Kotani,
- Tomoya IshizukaTomoya IshizukaDepartment of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, JapanMore by Tomoya Ishizuka,
- Yoshihiro KonYoshihiro KonInterdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, JapanMore by Yoshihiro Kon, and
- Takahiko Kojima*Takahiko Kojima*E-mail: [email protected] (T.K.).Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, JapanMore by Takahiko Kojima
Abstract
We have designed and synthesized a hetero-dinuclear RuII–CoII complex with a dinucleating ligand inspired by hetero-dinuclear active sites of metalloenzymes. A synergistic effect between the adjacent RuII and CoII sites has been confirmed in catalytic olefin hydrogenation by the complex, exhibiting a much higher turnover number than those of mononuclear RuII or CoII complexes as the components. A RuII-hydrido species was detected by 1H NMR and electrospray ionization (ESI)-time-of-flight (TOF)-MS measurements as an intermediate to react with olefins, and CoII-bound methanol was suggested to act as a proton source.
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- Dachao Hong, Yoshihiro Shimoyama, Yuji Ohgomori, Ryoichi Kanega, Hiroaki Kotani, Tomoya Ishizuka, Yoshihiro Kon, Yuichiro Himeda, Takahiko Kojima. Cooperative Effects of Heterodinuclear IrIII–MII Complexes on Catalytic H2 Evolution from Formic Acid Dehydrogenation in Water. Inorganic Chemistry 2020, 59 (17) , 11976-11985. https://doi.org/10.1021/acs.inorgchem.0c00812