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通过使用共反应物对单个金纳米团簇进行动态表面重构可实现颜色可调的电化学发光。

Dynamic surface reconstruction of individual gold nanoclusters by using a co-reactant enables color-tunable electrochemiluminescence.

作者信息

Lei Yan-Mei, Wu Di, Pan Mei-Chen, Tao Xiu-Li, Zeng Wei-Jia, Gan Li-Yong, Chai Ya-Qin, Yuan Ruo, Zhuo Ying

机构信息

Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University Chongqing 400715 China

Institute of Molecular Medicine, Renji Hospital, School of Medicine, Shanghai Jiao Tong University Shanghai 200127 China.

出版信息

Chem Sci. 2024 Jan 16;15(9):3255-3261. doi: 10.1039/d3sc06148e. eCollection 2024 Feb 28.

DOI:10.1039/d3sc06148e
PMID:38425534
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10901519/
Abstract

Here we report for the first time the phenomenon of continuously color-tunable electrochemiluminescence (ECL) from individual gold nanoclusters (Au NCs) confined in a porous hydrogel matrix by adjusting the concentration of the co-reactant. Specifically, the hydrogel-confined Au NCs exhibit strong dual-color ECL in an aqueous solution with triethylamine (TEA) as a co-reactant, with a record-breaking quantum yield of 95%. Unlike previously reported Au NCs, the ECL origin of the hydrogel-confined Au NCs is related to both the Au(0) kernel and the Au(i)-S surface. Surprisingly, the surface-related ECL of Au NCs exhibits a wide color-tunable range of 625-829 nm, but the core-related ECL remains constant at 489 nm. Theoretical and experimental studies demonstrate that the color-tunable ECL is caused by the dynamic surface reconstruction of Au NCs and TEA radicals. This work opens up new avenues for dynamically manipulating the ECL spectra of core-shell emitters in biosensing and imaging research.

摘要

在此，我们首次报道了通过调节共反应物浓度，在限域于多孔水凝胶基质中的单个金纳米簇（Au NCs）实现连续颜色可调的电化学发光（ECL）现象。具体而言，水凝胶限域的Au NCs在以三乙胺（TEA）作为共反应物的水溶液中表现出强烈的双色ECL，量子产率高达95%，打破了记录。与先前报道的Au NCs不同，水凝胶限域的Au NCs的ECL起源与Au(0)内核和Au(i)-S表面均有关。令人惊讶的是，Au NCs的表面相关ECL呈现出625 - 829 nm的宽颜色可调范围，但内核相关ECL在489 nm处保持恒定。理论和实验研究表明，颜色可调的ECL是由Au NCs和TEA自由基的动态表面重构引起的。这项工作为在生物传感和成像研究中动态操纵核壳发射体的ECL光谱开辟了新途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/cfaf8a40661b/d3sc06148e-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/daa0c7356a68/d3sc06148e-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/daae950bf584/d3sc06148e-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/5078eea35157/d3sc06148e-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/7f896ec51184/d3sc06148e-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/cfaf8a40661b/d3sc06148e-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/daa0c7356a68/d3sc06148e-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/daae950bf584/d3sc06148e-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/5078eea35157/d3sc06148e-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/7f896ec51184/d3sc06148e-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b08e/10901519/cfaf8a40661b/d3sc06148e-f5.jpg

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