期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 13, 页码 4555-4564出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b00710
关键词
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资金
- Leverhulme Trust [F/08 699/E]
- OUP John Fell Fund
- ARC
- EU (Marie Curie grant) [PIEF-GA-2013-626441]
- NSERC
- EPSRC [EP/L025000/1, EP/K014714/1]
- Engineering and Physical Sciences Research Council [EP/K014668/1, EP/K014714/1, EP/L025000/1] Funding Source: researchfish
- EPSRC [EP/K014714/1, EP/L025000/1, EP/K014668/1] Funding Source: UKRI
By employing strongly sigma-donating boryl ancillary ligands, the oxidative addition of H-2 to a single site Sn-II system has been achieved for the first time, generating (boryl)(2)SnH2. Similar chemistry can also be achieved for protic and hydridic E-H bonds (N-H/O-H, Si-H/B-H, respectively). In the case of ammonia (and water, albeit more slowly), E-H oxidative addition can be shown to be followed by reductive elimination to give an N- (or O-)borylated product. Thus, in stoichiometric fashion, redox-based bond cleavage/formation is demonstrated for a single main group metal center at room temperature. From a mechanistic viewpoint, a two-step coordination/proton transfer process for N-H activation is shown to be viable through the isolation of species of the types Sn(boryl)(2)center dot NH3 and [Sn(boryl)(2)(NH2)](-) and their onward conversion to the formal oxidative addition product Sn(boryl)(2)(H)(NH2).
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