Voltage-driven control of single-molecule keto-enol equilibrium in a two-terminal junction system

Tang，Chun1,2; Stuyver，Thijs3,4; Lu，Taige1; Liu，Junyang1; Ye，Yiling1; Gao，Tengyang1; Lin，Luchun1; Zheng，Jueting1; Liu，Wenqing1; Shi，Jia1; Shaik，Sason3; Xia，Haiping1,2; Hong，Wenjing1

2023-12-01

10.1038/s41467-023-39198-7

Nature Communications   影响因子和分区

2041-1723

Keto-enol tautomerism, describing an equilibrium involving two tautomers with distinctive structures, provides a promising platform for modulating nanoscale charge transport. However, such equilibria are generally dominated by the keto form, while a high isomerization barrier limits the transformation to the enol form, suggesting a considerable challenge to control the tautomerism. Here, we achieve single-molecule control of a keto-enol equilibrium at room temperature by using a strategy that combines redox control and electric field modulation. Based on the control of charge injection in the single-molecule junction, we could access charged potential energy surfaces with opposite thermodynamic driving forces, i.e., exhibiting a preference for the conducting enol form, while the isomerization barrier is also significantly reduced. Thus, we could selectively obtain desired and stable tautomers, which leads to significant modulation of the single-molecule conductance. This work highlights the concept of single-molecule control of chemical reactions on more than one potential energy surface.

SCI

英语

NI论文

通讯

National Natural Science Foundation of China-Yunnan Joint Fund[21722305];

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:001026336000013

NATURE PORTFOLIO

2-s2.0-85162678345

Scopus

1.State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen,361005,China
2.Shenzhen Grubbs Institute,Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
3.Institute of Chemistry,The Hebrew University,Jerusalem,Edmond J. Safra Campus at Givat Ram,91904,Israel
4.Ecole Nationale Supérieure de Chimie de Paris,Université PSL,CNRS,Institute of Chemistry for Life and Health Sciences,Paris,75 005,France

Tang，Chun,Stuyver，Thijs,Lu，Taige,et al. Voltage-driven control of single-molecule keto-enol equilibrium in a two-terminal junction system[J]. Nature Communications,2023,14(1).

Tang，Chun.,Stuyver，Thijs.,Lu，Taige.,Liu，Junyang.,Ye，Yiling.,...&Hong，Wenjing.(2023).Voltage-driven control of single-molecule keto-enol equilibrium in a two-terminal junction system.Nature Communications,14(1).

Tang，Chun,et al."Voltage-driven control of single-molecule keto-enol equilibrium in a two-terminal junction system".Nature Communications 14.1(2023).