Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c07920
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Funding
- National Science Foundation [CHE-1855641, CHE-2153978, CHE-2134792]
- NSF Major Research Instrumentation (MRI) [1827968]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1827968] Funding Source: National Science Foundation
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In this study, the mechanism of ammonia activation by a carbene-stabilized dithiolene zwitterion was investigated through experimental and computational methods. The synthesis of 4• and 5 was achieved, and it represents the first metal-free ammonia activation via hydrogen atom transfer.
A carbene-stabilized dithiolene zwitterion (3) activates ammonia, affording 4 & BULL; and 5, through both single-electron transfer (SET) and hydrogen atom transfer (HAT). Reaction products were characterized spectroscopically and by single-crystal Xray diffraction. The mechanism of the formation of 4 & BULL; and 5 was probed by experimental and computational methods. This discovery is the first example of metal-free ammonia activation via HAT.
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