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Single-atom catalysts enable the first C-C bond formation in Heck reactions. Novel platinum-carbon sites and a base effect facilitate this complex catalytic process.

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Area of Science:

  • Heterogeneous catalysis
  • Organometallic chemistry
  • Materials science

Background:

  • Single-atom catalysts (SACs) offer high reactivity and selectivity by isolating metal atoms.
  • SACs have been limited to small-molecule reactions, with challenges in complex bond-forming reactions like cross-coupling.

Purpose of the Study:

  • To develop a single-atom catalyst for C-C bond formation in cross-coupling reactions.
  • To investigate the mechanism of a heterogeneous single-atom platinum-catalyzed Heck reaction.

Main Methods:

  • Supercritical carbon dioxide-assisted synthesis of a heterogeneous single-atom platinum catalyst.
  • Quantum mechanical computations to elucidate the reaction mechanism.
  • Experimental investigation of the Heck reaction using the developed SAC.

Main Results:

  • Achieved the first C-C bond-forming migratory insertion on a single-atom catalyst (SAC).
  • Identified a novel platinum-carbon (PtC4) coordination site with an unexpected base effect.
  • Demonstrated transient modulation of the coordination environment by a base, enabling sterically hindered migratory insertion.

Conclusions:

  • SACs can be designed for complex bond-forming reactions previously inaccessible.
  • The novel PtC4 site and base modulation offer new strategies for catalyst design.
  • This work opens avenues for applying migratory insertion chemistry to heterogeneous SACs.