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A new strategy for the generation of the active Pd‐alkyl species from aminal via C—N bond activation has been established, in which the formation of zwitterionic intermediate through aza‐Michael addition of aminal to nitrodienes or dienones is identified as a key step for the activation of the C—N bond. The efficient strategy has enabled a new palladium‐catalyzed α‐aminomethylation of nitrodienes...
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