Pre-oxidation of Gold Nanoclusters Results in a 66 % Anodic Electrochemiluminescence Yield and Drives Mechanistic Insights
Pre-oxidation of Gold Nanoclusters Results in a 66 % Anodic Electrochemiluminescence Yield and Drives Mechanistic Insights
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预氧化%20of%20金%20纳米团簇%20结果%20in%20a%2066-%%20阳极%20电化学发光%20产量%20和%20驱动%20机械%20见解
DOI：
10.1002/anie.201905007
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发表时间：
2019-07-18
影响因子：
16.6
通讯作者：
Liu, Juewen
中科院分区：
文献类型：
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作者：
Peng, Huaping;Huang, Zhongnan;Liu, Juewen
金纳米团簇（AuNCs）具有良好的稳定性、近红外发射和生物相容性，是一种极具吸引力的电化学发光材料。然而，它们的ECL量子产率相对较低，我们有限的基本理解阻碍了这一参数的合理改善。在此，我们报告了配体稳定的金纳米粒子的电化学发光的急剧增强，通过在电极上预氧化与三乙胺（TEA）作为共反应物。L-甲硫氨酸稳定的AuNC导致66%的创纪录高ECL产率。这种策略被成功地扩展到其他AuNCs，并且对于允许更有效的电子转移的配体壳层更有效。此外，预氧化ECL的激发需要比常规方法更低的电位，并且不需要额外的仪器。这项工作为解决基于AuNC的ECL探针的挑战性问题开辟了途径，丰富了基本的理解，大大拓宽了其潜在的应用。
Gold nanoclusters (AuNCs) are attractive electrochemiluminescence (ECL) emitters because of their excellent stability, near IR emission, and biocompatibility. However, their ECL quantum yield is relatively low, and our limited fundamental understanding has hindered rational improvement of this parameter. Herein, we report drastic enhancement of the ECL of ligand-stabilized AuNCs by on-electrode pre-oxidation with triethylamine (TEA) as a co-reactant. The l-methionine-stabilized AuNCs resulted in a record high ECL yield of 66 %. This strategy was successfully extended to other AuNCs, and it is more effective for ligand shells that allow more effective electron transfer. In addition, excitation of the pre-oxidized ECL required a lower potential than conventional methods, and no additional instrument was required. This work opens avenues for solving a challenging problem of AuNC-based ECL probes and enriches fundamental understanding, greatly broadening their potential applications.