College of Chemistry, Jilin University, Changchun, Jilin 130012, China.
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China.
Anal Chem. 2024 Jan 9;96(1):514-521. doi: 10.1021/acs.analchem.3c04645. Epub 2023 Dec 25.
Modulating the photon emission of the luminophore for boosting chemiluminescence (CL) response is very crucial for the construction of highly sensitive sensors via the introduction of functionalized materials. Herein, the integration of the emitter and coreactant accelerator into one entity is realized by simply assembling cucurbit[7]uril (CB[7]) on the surface of gold nanoparticles (AuNPs) through simple assembly via a Au-O bond. The loaded CB[7] on the AuNPs improves their catalytic capacity for the generation of hydroxyl radicals(OH). Moreover, the host-guest recognition interaction between luminol and CB[7] enables the capture of luminol on AuNPs efficiently. Also, the intramolecular electron-transfer reaction between the luminol and OH enables the CL response more effectively in the entity, which greatly boosts photon emission ca 100 folds compared with the individual luminol/HO. The host-guest recognition between luminol and CB[7] is revealed by Fourier transform infrared spectroscopy, electrochemical, and thermogravimetric characterization. Moreover, the proposed CL system is successfully used for the sensitive and selective determination of dopamine (DA) based on a synergistic quenching mechanism including the competition quenching and radical-scavenging effect from DA. The present amplified strategy by integrating recognized and amplified elements within one entity simplifies the sensing process and holds great potential for sensitive analysis based on the self-enhanced strategies.
调制发光体的光子发射以增强化学发光(CL)响应对于通过引入功能化材料构建高灵敏度传感器非常重要。在此,通过简单地通过 Au-O 键将葫芦[7]脲(CB[7])组装在金纳米粒子(AuNPs)的表面上,将发射器和共反应物加速器集成到一个实体中。负载在 AuNPs 上的 CB[7]提高了它们生成羟基自由基(OH)的催化能力。此外,鲁米诺和 CB[7]之间的主体-客体识别相互作用使鲁米诺能够有效地捕获 AuNPs 上的鲁米诺。此外,鲁米诺和 OH 之间的分子内电子转移反应使实体中的 CL 响应更有效,与单独的鲁米诺/HO 相比,光子发射大大提高了 ca 100 倍。鲁米诺和 CB[7]之间的主体-客体识别通过傅里叶变换红外光谱、电化学和热重分析得到证实。此外,该提议的 CL 系统成功地用于基于协同猝灭机制(包括来自 DA 的竞争猝灭和自由基清除效应)的灵敏和选择性测定多巴胺(DA)。通过在一个实体中整合识别和放大元件,这种放大策略简化了传感过程,并基于自增强策略在灵敏分析方面具有很大的潜力。