Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 26, Issue 53, Pages 12168-12179Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202002013
Keywords
copper; metal-metal cooperation; metal-metal interactions; palladium; Sonogashira coupling
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Funding
- Spanish MINECO [CTQ2017-87889-P, PGC2018-100818-A-I00, RyC-2016-19930]
- JSPS KAKENHI [16F16038]
- OIST
- Grants-in-Aid for Scientific Research [16F16038] Funding Source: KAKEN
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Cooperation between two different metals plays a crucial role in many synergistic catalytic reactions, such as the Sonogashira C-C cross-coupling reaction, where an interaction between the Pd and Cu centers is proposed in the transmetalation step. Although several heterobimetallic Pd/Cu complexes were proposed as structural models of the active species in Sonogashira coupling, the detailed understanding of the metal-metal cooperation in transmetalation is still lacking in current systems. In this work, we report a stepwise and systematic approach to building heteromultimetallic Pd/Cu assemblies as a tool to study metal-metal cooperativity. We obtained fully characterized Pd/Cu multimetallic assemblies that show reactivity in alkyne activation, formation of catalytically relevant aryl/acetylide species, and C-C elimination, serving as functional models for Sonogashira reaction intermediates. The combined experimental and DFT studies highlight the importance of ligand-controlled coordination geometry, metal-metal distances and dynamics of the multimetallic assembly for transmetalation step.
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