Palladium-Catalyzed Formal anti -Markovnikov Hydroamidation of 1,3-Dienes with Disilane via 1,4-Silylamidation/Protodesilylation

Abstract Hydroamidation of 1,3-dienes with carboxamides remains underdeveloped, particularly for anti-Markovnikov selectivity. We report a disilane-mediated silicon relay strategy in which palladium-catalyzed 1,4-silylamidation generates an allylsilane intermediate that undergoes protodesilylation to furnish the first formal anti-Markovnikov hydroamidation of 1,3-dienes. Suppression of protodesilylation selectively affords 1,4-silylamidation products. Experimental and computational studies clarify the origin of the divergent reaction outcomes.

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Publication Details

Journal
Organic Letters
Published
2026-09-25
DOI
https://doi.org/10.1021/acs.orglett.6c03575
Primary Topic
Organoboron and organosilicon chemistry
Type
article
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article

Palladium-Catalyzed Formal anti -Markovnikov Hydroamidation of 1,3-Dienes with Disilane via 1,4-Silylamidation/Protodesilylation

Nobuki Katayama, Kazuhiko Semba, Tetsuaki Fujihara, Hiroki Yamaguchi et al.
Organic Letters
Organoboron and organosilicon chemistry
article

Palladium-Catalyzed Formal anti -Markovnikov Hydroamidation of 1,3-Dienes with Disilane via 1,4-Silylamidation/Protodesilylation

Nobuki Katayama, Kazuhiko Semba, Tetsuaki Fujihara, Hiroki Yamaguchi, Yasushi Obora, Kazuki Tabaru, Tsz-Chun Chan
article en

Abstract

Abstract Hydroamidation of 1,3-dienes with carboxamides remains underdeveloped, particularly for anti-Markovnikov selectivity. We report a disilane-mediated silicon relay strategy in which palladium-catalyzed 1,4-silylamidation generates an allylsilane intermediate that undergoes protodesilylation to furnish the first formal anti-Markovnikov hydroamidation of 1,3-dienes. Suppression of protodesilylation selectively affords 1,4-silylamidation products. Experimental and computational studies clarify the origin of the divergent reaction outcomes.

Organic Letters
Kansai University (JP)
Openalex Percentile: Top 22%
Organoboron and organosilicon chemistry
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Palladium-Catalyzed Formal anti -Markovnikov Hydroamidation of 1,3-Dienes with Disilane via 1,4-Silylamidation/Protodesilylation — Nobuki Katayama, Kazuhiko Semba, et al. · Organic Letters (2026) | TGRS Research Map | TGRS