TY - JOUR
T1 - Catalytic Oxidative Deamination by Water with H2Liberation
AU - Tang, Shan
AU - Rauch, Michael
AU - Montag, Michael
AU - Diskin-Posner, Yael
AU - Ben-David, Yehoshoa
AU - Milstein, David
N1 - Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/12/9
Y1 - 2020/12/9
N2 - Selective oxidative deamination has long been considered to be an important but challenging transformation, although it is a common critical process in the metabolism of bioactive amino compounds. Most of the synthetic methods developed so far rely on the use of stoichiometric amounts of strong and toxic oxidants. Here we present a green and efficient method for oxidative deamination, using water as the oxidant, catalyzed by a ruthenium pincer complex. This unprecedented reaction protocol liberates hydrogen gas and avoids the use of sacrificial oxidants. A wide variety of primary amines are selectively transformed to carboxylates or ketones in good to high yields. It is noteworthy that mechanistic experiments and DFT calculations indicate that in addition to serving as the oxidant, water also plays an important role in assisting the hydrogen liberation steps involved in amine dehydrogenation.
AB - Selective oxidative deamination has long been considered to be an important but challenging transformation, although it is a common critical process in the metabolism of bioactive amino compounds. Most of the synthetic methods developed so far rely on the use of stoichiometric amounts of strong and toxic oxidants. Here we present a green and efficient method for oxidative deamination, using water as the oxidant, catalyzed by a ruthenium pincer complex. This unprecedented reaction protocol liberates hydrogen gas and avoids the use of sacrificial oxidants. A wide variety of primary amines are selectively transformed to carboxylates or ketones in good to high yields. It is noteworthy that mechanistic experiments and DFT calculations indicate that in addition to serving as the oxidant, water also plays an important role in assisting the hydrogen liberation steps involved in amine dehydrogenation.
UR - http://www.scopus.com/inward/record.url?scp=85097579480&partnerID=8YFLogxK
U2 - 10.1021/jacs.0c10826
DO - 10.1021/jacs.0c10826
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C2 - 33237749
AN - SCOPUS:85097579480
SN - 0002-7863
VL - 142
SP - 20875
EP - 20882
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 49
ER -