Accelerated proton dissociation in an excited state induces superacidic microenvironments around graphene quantum dots

Yongqiang Li, Siwei Yang (), Wancheng Bao, Quan Tao, Xiuyun Jiang, Jipeng Li, Peng He, Gang Wang, Kai Qi (), Hui Dong (), Guqiao Ding () and Xiaoming Xie
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Yongqiang Li: Chinese Academy of Sciences
Siwei Yang: Chinese Academy of Sciences
Wancheng Bao: Chinese Academy of Sciences
Quan Tao: Chinese Academy of Sciences
Xiuyun Jiang: Chinese Academy of Sciences
Jipeng Li: Shanghai Ninth People’s Hospital
Peng He: Chinese Academy of Sciences
Gang Wang: Ningbo University
Kai Qi: University of Chinese Academy of Sciences
Hui Dong: Chinese Academy of Sciences
Guqiao Ding: Chinese Academy of Sciences
Xiaoming Xie: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Investigating proton transport at the interface in an excited state facilitates the mechanistic investigation and utilization of nanomaterials. However, there is a lack of suitable tools for in-situ and interfacial analysis. Here we addresses this gap by in-situ observing the proton transport of graphene quantum dots (GQDs) in an excited state through reduction of magnetic resonance relaxation time. Experimental results, utilizing 0.1 mT ultra-low-field nuclear magnetic resonance relaxometry compatible with a light source, reveal the light-induced proton dissociation and acidity of GQDs’ microenvironment in the excited state (Hammett acidity function: –13.40). Theoretical calculations demonstrate significant acidity enhancement in –OH functionalized GQDs with light induction ( $${{\mathrm{p}}}{K}_{{\text{a}}}^{*}$$ p K a * = –4.62, stronger than that of H2SO4). Simulations highlight the contributions of edge and phenolic –OH groups to proton dissociation. The light-induced superacidic microenvironment of GQDs benefits functionalization and improves the catalytic performances of GQDs. Importantly, this work advances the understanding of interfacial properties of light-induced sp2–sp3 carbon nanostructure and provides a valuable tool for exploring catalyst interfaces in photocatalysis.

Date: 2024
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DOI: 10.1038/s41467-024-50982-x

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