期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c07290
关键词
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资金
- JSPS fellowship [20J22190]
- JSPS KAKENHI [JP18K05144, JP18H01940, JP20H04808, JP21K18978, JP21K04996, JP22H05146, JP22H00335]
- JST PRESTO program [JPMJPR15S7, JPMJPR17S3]
- JST CREST [JPMJCR15P5]
- MEXT project Integrated Research on Chemical Synthesis
- Integrated Research Consortium on Chemical Sciences
- World Research Unit (B-1) at Nagoya University Reaction Infography (R-ing)
- Iketani Science and Technology Foundation
- Hori Science and Arts Foundation
- Chubei Itoh Foundation
- MEXT, Japan [JPMXP09S19MS1052, JPMXP09S20MS1064, JPMXP09S21MS1061, JPMXP1222MS1011]
- Research Center for Computational Science, Okazaki, Japan [21-IMS-C261]
- Deutsche Forschungsgemeinschaft [SFB 858, SFB 1459]
A coordination-induced trigger for catalytic activity is proposed on an N-heterocyclic carbene (NHC)-decorated ceria catalyst incorporating Cr and Rh (ICy-r-Cr0.19Rh0.06CeOz). The ICy-bearing Rh nanoclusters were found to be the key active species, and the ICy controlled the adsorption sites of the phenyl group on the Rh nanocluster to promote the C-C bond formation.
A coordination-induced trigger for catalytic activity is proposed on an N-heterocyclic carbene (NHC)-decorated ceria catalyst incorporating Cr and Rh (ICy-r-Cr0.19Rh0.06CeOz). ICy-r-Cr0.19Rh0.06CeOz was prepared by grafting 1,3-dicyclohexylimidazol-2-ylidene (ICy) onto H2-reduced Cr0.19Rh0.06CeOz (r-Cr0.19Rh0.06CeOz) surfaces, which went on to exhibit substantial catalytic activity for the 1,4-arylation of cyclohexenone with phenylboronic acid, whereas r-Cr0.19Rh0.06CeOz without ICy was inactive. FT-IR, Rh K-edge XAFS, XPS, and photoluminescence spectroscopy showed that the ICy carbene-coordinated Rh nanoclusters were the key active species. The coordination-induced trigger for catalytic activity on the ICy-bearing Rh nanoclusters could not be attributed to electronic donation from ICy to the Rh nanoclusters. DFT calculations suggested that ICy controlled the adsorption sites of the phenyl group on the Rh nanocluster to promote the C-C bond formation of the phenyl group and cyclohexenone.
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