Enzyme-activatable charge transfer in gold nanoclusters

Deng, Hao-Hua; Huang, Kai-Yuan; Zhong, Yu; Li, Ye; Huang, Hong-Xiang; Fang, Xiang-Yu; Sun, Wei-Ming; Yao, Qiaofeng; Chen, Wei; Xie, Jianping

doi:10.1039/d4sc01509f

Chem. Sci.

2024

DOI: 10.1039/d4sc01509f

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Enzyme-activatable charge transfer in gold nanoclusters

Hao-Hua Deng,

Kai-Yuan Huang,

Yu Zhong

et al.

Abstract: We report herein a new kind of water-soluble gold nanoclusters (AuNCs) for enzyme-activatable charge transfer, based on the ligand engineering of AuNCs with 6-mercaptopurine ribonucleoside (MPR).

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The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

Huang,

Chen,

Wang

et al. 2024

Angewandte Chemie

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Comprehending the underlying factors that govern photoluminescence (PL) in metal nanoclusters (NCs) under physiological conditions remains a highly intriguing and unresolved challenge, particularly for their biomedical applications. In this study, we evaluate the critical role of excited‐state proton‐coupled electron transfer in the emission of metal NCs. Our findings demonstrate that hydronium ion (H3O+) binding can trigger a nonlinear, pH‐dependent excited‐state concerted electron proton transfer (CEPT) reaction. This involves simultaneous electron transfer from the Au(0) core to the Au(I)‐ATT (ATT denotes 6‐aza‐2‐thiothymidine) surface and proton transfer from H3O+ to the ATT ligand in a single step, greatly promoting vibrations and rotations of the Au(I)‐ATT surface, resulting in substantial PL quenching of Au10(ATT)6 NCs. Further analyses show that the unique CEPT dynamics are strongly influenced by the opposing effects of increased reorganization energy and a larger pre‐exponential factor on the electron transfer rate. Moreover, the proposed excited‐state CEPT process is found to be prevalent in core‐shell relaxation metal NCs, such as Au25(SR)18 (SR denotes thiolate) NCs, and serves as an important factor in limiting their PL emission. By simply controlling the pKa of the ligands, the emission performance of Au25(SR)18 can be easily regulated in physiological environments.

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The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

Huang,

Chen,

Wang

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

Huang,

Chen,

Wang

et al. 2024

Angew Chem Int Ed

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Fluorescent metal nanoclusters for explosive detection: A review

Gao,

Zhao,

Shang

2024

TrAC Trends in Analytical Chemistry

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Enzyme-activatable charge transfer in gold nanoclusters

Abstract: We report herein a new kind of water-soluble gold nanoclusters (AuNCs) for enzyme-activatable charge transfer, based on the ligand engineering of AuNCs with 6-mercaptopurine ribonucleoside (MPR).

Cited by 3 publications

References 75 publications

The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

The Hidden Mechanism: Excited‐State Proton‐Electron Pair Transfer in Metal Nanocluster Emission

Fluorescent metal nanoclusters for explosive detection: A review

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