Single-Electron Catalysis of Reversible Cycloadditions under Nanoconfinement

Electron transfer (ET) is crucial in many chemical reactions, but its mechanism and role are hardly understood in nanobiotechnology due to the complexity of reaction species and pathways involved. By modulating and monitoring electron behavior at the single-molecule level, we can better understand the fundamental mechanisms and ways to control them for technological use. Here, we unravel a mechanism of single-electron catalysis under positively charged nanoconfinement. We demonstrate that both (2 + 2) and (4 + 4) cycloadditions can be catalyzed reversibly by a single electron. Key reaction pathways are discovered by monitoring sequential electrical signals in the cycloadditions through advanced single-molecule detection platforms. Experimental and theoretical results consistently demonstrate that combining single ET processes with nanoconfinement involving cucurbit[8]uril can lower the reaction energy barrier and promote reversible cycloaddition. Moreover, we show that the bias voltage can fine-tune ET processes and chemical equilibria in bond formation and cleavage. Our results provide a novel approach to elucidate, modulate, and design electron-involved reactions and functionalized devices.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-02-06
DOI
https://doi.org/10.1021/jacs.4c18064
Citations
11
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
4.00

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article

Single-Electron Catalysis of Reversible Cycloadditions under Nanoconfinement

Chuancheng Jia, Agostino Migliore, Suhang He, J. Fraser Stoddart et al.
11 citations
Journal of the American Chemical Society
CO2 Reduction Techniques and Catalysts
4.00
article

Single-Electron Catalysis of Reversible Cycloadditions under Nanoconfinement

Chuancheng Jia, Agostino Migliore, Suhang He, J. Fraser Stoddart, Kendall N. Houk, Chunyan Gao, Xin Zhu, Jiawen Cao, Yang Jiao, Xuefeng Guo, Baoyi Wang, Jinlong Yang, Hongliang Chen, Xingxing Li, Chen Yang, Yanwei Li, Jinying Wang, C. L. Yang
article en
11 citations

Abstract

Electron transfer (ET) is crucial in many chemical reactions, but its mechanism and role are hardly understood in nanobiotechnology due to the complexity of reaction species and pathways involved. By modulating and monitoring electron behavior at the single-molecule level, we can better understand the fundamental mechanisms and ways to control them for technological use. Here, we unravel a mechanism of single-electron catalysis under positively charged nanoconfinement. We demonstrate that both (2 + 2) and (4 + 4) cycloadditions can be catalyzed reversibly by a single electron. Key reaction pathways are discovered by monitoring sequential electrical signals in the cycloadditions through advanced single-molecule detection platforms. Experimental and theoretical results consistently demonstrate that combining single ET processes with nanoconfinement involving cucurbit[8]uril can lower the reaction energy barrier and promote reversible cycloaddition. Moreover, we show that the bias voltage can fine-tune ET processes and chemical equilibria in bond formation and cleavage. Our results provide a novel approach to elucidate, modulate, and design electron-involved reactions and functionalized devices.

Journal of the American Chemical SocietyVol. 147(7)
Northwestern University (US), University of Science and Technology of China (CN), University of Padua (IT), Shandong University (CN), University of California, Los Angeles (US), Zhejiang University of Science and Technology (CN), Peking University (CN), Nankai University (CN), University of California System (US), Hefei National Center for Physical Sciences at Nanoscale (CN), City University of Hong Kong, Shenzhen Research Institute (CN), Beijing National Laboratory for Molecular Sciences (CN), Microscale (United States) (US), Zhejiang University (CN), University of Hong Kong (HK)
National Natural Science Foundation of China, Youth Innovation Promotion Association of the Chinese Academy of Sciences, National Key Research and Development Program of China, Beijing National Laboratory for Molecular Sciences
Openalex Percentile: Top 6%
CO2 Reduction Techniques and Catalysts
4.00
DOISourceOpenAlex
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