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Stable Discrete Pt-1(0) in Crown Ether with Ultra-High Hydrosilylation Activity
Liu, Kairui1; Shen, Xing1,2; Bai, Shi3; Zhang, Z. Conrad1
2019-11-26
Source PublicationCHEMCATCHEM
ISSN1867-3880
Pages7
AbstractObtaining reduced discrete metal atoms that are stable in liquid solvents by in-situ reduction of an ionic metal precursor has been a challenge until recently. A liquid surfactant polydimethylsiloxane-polyethylene glycol (PDMS-PEG) enabled the synthesis of stable discrete platinum atoms (Pt-1) by reducing Pt(IV) and Pt(II) salts. Here we report the successful preparation of discrete mononuclear platinum atoms (Pt-1) in a crown ether, [15]crown-5, as a structurally much simpler solvent, and the prepared Pt-1@[15]crown-5 was demonstrated for ultra-high catalytic activity and selectivity in hydrosilylation reactions. A combination of spectroscopic characterizations proves the reduced Pt species is Pt-1(0) with partially positive charge. Pt-195 NMR and DFT calculation indicate the Pt-1(0) is stabilized by the pseudo octahedral structure of ([15]crown-5)PtCl2-H2+ involving two adjacent oxygens from the crown ether ring, although the oxygens in the crown ether ring have been known to host and stabilize certain metal cations. The Pt-1@[15]crown-5 shows ultrahigh activity (TOF of 8.3x10(8) h(-1)) with excellent terminal adducts selectivity in catalytic olefin hydrosilylation. This catalyst was found to be highly stable under hydrosilylation conditions. For examples, the turnover number (TON) exceeded 1.0x10(9) for hydrosilylation between 1-octene and (Me3SiO)(2)MeSiH without showing sign of deactivation; the TON exceeded 2.0x10(8) while the catalyst remained active for a catalytically more demanding reaction between styrene and (Me3SiO)(2)MeSiH.
KeywordCrown Ether Density Functional Calculations Hydrosilylation Metal Atom Catalyst Platinum
DOI10.1002/cctc.201901577
Language英语
WOS KeywordCATALYTIC HYDROSILYLATION ; PLATINUM(0)-CARBENE COMPLEXES ; COORDINATION CHEMISTRY ; PLATINUM ; NANOPARTICLES ; EFFICIENT ; NMR ; OXIDATION ; SIZE
Funding Project"Global Expert" program of China ; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences ; National Institute of General Medical Sciences-NIGMS from the National Institutes of Health[5 P30 GM110758-02]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
Funding Organization"Global Expert" program of China ; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences ; National Institute of General Medical Sciences-NIGMS from the National Institutes of Health
WOS IDWOS:000498435300001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/38380
Collection中国科学院过程工程研究所
Corresponding AuthorBai, Shi; Zhang, Z. Conrad
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, Beijing 100049, Peoples R China
3.Univ Delaware, Dept Chem & Biochem, Newark, DE 19716 USA
Recommended Citation
GB/T 7714
Liu, Kairui,Shen, Xing,Bai, Shi,et al. Stable Discrete Pt-1(0) in Crown Ether with Ultra-High Hydrosilylation Activity[J]. CHEMCATCHEM,2019:7.
APA Liu, Kairui,Shen, Xing,Bai, Shi,&Zhang, Z. Conrad.(2019).Stable Discrete Pt-1(0) in Crown Ether with Ultra-High Hydrosilylation Activity.CHEMCATCHEM,7.
MLA Liu, Kairui,et al."Stable Discrete Pt-1(0) in Crown Ether with Ultra-High Hydrosilylation Activity".CHEMCATCHEM (2019):7.
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