4.8 Article

Selectivity in single-molecule reactions by tip-induced redox chemistry

期刊

SCIENCE
卷 377, 期 6603, 页码 298-301

出版社

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abo6471

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资金

  1. ERC Synergy Grant MolDAM [951519]
  2. ERC Consolidator Grant AMSEL [682144]
  3. European FET-OPEN project SPRING [863098]
  4. Spanish Agencia Estatal de Investigacion [PID2019-107338RB-C62, PID2019-110037GB-I00, PCI2019-111933-2]
  5. Xunta de Galicia (Centro de Investigacion de Galicia accreditation 2019-2022) [ED431G 2019/03]
  6. European Regional Development Fund (ERDF)
  7. European Research Council (ERC) [682144, 951519] Funding Source: European Research Council (ERC)

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This work demonstrates reversible and selective bond formation and dissociation promoted by tip-induced reduction-oxidation reactions on a surface. Molecular rearrangements leading to different constitutional isomers are selected by the polarity and magnitude of applied voltage pulses from the tip. Density functional theory calculations reveal the importance of the energy landscape of the isomers in different charge states for rationalizing the selectivity.
Controlling selectivity of reactions is an ongoing quest in chemistry. In this work, we demonstrate reversible and selective bond formation and dissociation promoted by tip-induced reduction-oxidation reactions on a surface. Molecular rearrangements leading to different constitutional isomers are selected by the polarity and magnitude of applied voltage pulses from the tip of a combined scanning tunneling and atomic force microscope. Characterization of voltage dependence of the reactions and determination of reaction rates demonstrate selectivity in constitutional isomerization reactions and provide insight into the underlying mechanisms. With support of density functional theory calculations, we find that the energy landscape of the isomers in different charge states is important to rationalize the selectivity. Tip-induced selective single-molecule reactions increase our understanding of redox chemistry and could lead to novel molecular machines.

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