Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces

Cong Zhao; Jiazheng Diao; Zhao Liu; Jie Hao; Suhang He; Shaojia Li; Xingxing Li; Guangwu Li; Qiang Fu; Chuancheng Jia; Xuefeng Guo

doi:10.1038/s41467-024-53179-4

Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces

Nat Commun. 2024 Oct 13;15(1):8835. doi: 10.1038/s41467-024-53179-4.

Authors

Cong Zhao^#¹, Jiazheng Diao^#², Zhao Liu^#¹, Jie Hao¹, Suhang He¹, Shaojia Li¹, Xingxing Li^{2

3}, Guangwu Li^{4

5}, Qiang Fu^{6

7}, Chuancheng Jia⁸, Xuefeng Guo^{9

10}

Affiliations

¹ Center of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Center for New Organic Matter, Tianjin Key Laboratory of Micro-Scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, Tianjin, China.
² Hefei National Research Center for Physical Sciences at the Microscale, School of Future Technology, University of Science and Technology of China, Hefei, China.
³ Hefei National Laboratory, University of Science and Technology of China, Hefei, China.
⁴ Center of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Center for New Organic Matter, Tianjin Key Laboratory of Micro-Scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, Tianjin, China. [email protected].
⁵ Shenzhen Research, Institute of Nankai University, 16th Floor, Yantian Science & Technology Building, Shenzhen, China. [email protected].
⁶ Hefei National Research Center for Physical Sciences at the Microscale, School of Future Technology, University of Science and Technology of China, Hefei, China. [email protected].
⁷ Hefei National Laboratory, University of Science and Technology of China, Hefei, China. [email protected].
⁸ Center of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Center for New Organic Matter, Tianjin Key Laboratory of Micro-Scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, Tianjin, China. [email protected].
⁹ Center of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Center for New Organic Matter, Tianjin Key Laboratory of Micro-Scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, Tianjin, China. [email protected].
¹⁰ Beijing National Laboratory for Molecular Sciences, National Biomedical Imaging Center, College of Chemistry and Molecular Engineering, Peking University, Beijing, China. [email protected].

^# Contributed equally.

Abstract

Detecting chemical reaction dynamics at solid-liquid interfaces is important for understanding heterogeneous reactions. However, there is a lack of exploration of interface reaction dynamics from the single-molecule perspective, which can reveal the intrinsic reaction mechanism underlying ensemble experiments. Here, single-event protonation reaction dynamics at a solid-liquid interface are studied in-situ using single-molecule junctions. Molecules with amino terminal groups are used to construct single-molecule junctions. An interfacial cationic state present after protonation is discovered. Real-time electrical measurements are used to monitor the reversible reaction between protonated and deprotonated states, thereby revealing the interfacial reaction mechanism through dynamic analysis. The protonation reaction rate constant has a linear positive correlation with proton concentration, whereas the deprotonation reaction rate constant has a linear negative correlation. In addition, external mechanical forces can effectively regulate the protonation reaction process. This work provides a single-molecule perspective for exploring interface science, which will contribute to the development of heterogeneous catalysis and electrochemistry.

Abstract

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