网内电荷转移触发锆基金属有机框架纳米粒子的自电化学发光，用于分离共反应物的电位分辨多重免疫测定,Analytical Chemistry

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网内电荷转移触发锆基金属有机框架纳米粒子的自电化学发光，用于分离共反应物的电位分辨多重免疫测定
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-06-23 , DOI: 10.1021/acs.analchem.3c01820
Ping Zhang ₁ , Qirui Shen ₁ , Jiangru Wang ₁ , Miaomiao Yu ₁ , Qi Kang ₁ , Wei Zhang ₁ , Guizheng Zou ₂

Affiliation

在这项工作中，开发了一种电位分辨电化学发光 (ECL) 多重免疫分析 (MIA)，使用具有强烈自 ECL 的锆基金属有机框架 (MOF) 纳米粒子作为阳极 ECL 标签，CdTe 纳米晶体 (NC) 作为阴极ECL 标签。ECL 发光体 5,5'-(蒽-9,10-二基)二间苯二甲酸 (H ₄ ADIP) 和共反应物六亚甲基四胺 (HMT) 与 MOF 中的锆节点结合，得到 Zr-ADIP-HMT 纳米颗粒。_{受益于 H 4}氧化配体之间的网内电荷转移 (ICT)ADIP 和 HMT 通过氢键，将 Zr-ADIP-HMT 产生的强烈自 ECL 应用于无需外源阳极共反应剂的电位分辨 ECL MIA，这可以消除多重共反应剂和 CdTe NC 阳极 ECL 发射的有害影响。Zr-ADIP-HMT纳米颗粒内的ICT可以缩短电子传输路径并降低自由基中间传输的复杂性。_{Zr-ADIP-HMT 的 ECL 强度是 H 4} ADIP 和 HMT混合物的 18.6 倍。在潜在分辨的 ECL MIA 中，采用癌胚抗原和神经元特异性烯醇化酶这两种肺癌生物标志物作为模型分析物，检测限分别为 18 和 5.3 fg·mL ^–1，分别。双配体 Zr-ADIP-HMT 纳米粒子提供了使用基于 ICT 的自 ECL 发光体与分离的共反应物进行潜在分辨 ECL MIA 的概念证明。

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Intrareticular Charge Transfer Triggered Self-Electrochemiluminescence of Zirconium-Based Metal–Organic Framework Nanoparticles for Potential-Resolved Multiplex Immunoassays with Isolated Coreactants

In this work, a potential-resolved electrochemiluminescence (ECL) multiplex immunoassay (MIA) was developed using zirconium-based metal–organic framework (MOF) nanoparticles with intense self-ECL as an anodic ECL tag and CdTe nanocrystals (NCs) as a cathodic ECL tag. ECL luminophore 5,5′-(anthracene-9,10-diyl)diisophthalic acid (H₄ADIP) and coreactant hexamethylenetetramine (HMT) bound to zirconium nodes in the MOF, giving Zr-ADIP-HMT nanoparticles. Benefiting from the intrareticular charge transfer (ICT) between the oxidized ligands of H₄ADIP and HMT via hydrogen bonds, the intense self-ECL from Zr-ADIP-HMT was applied to the potential-resolved ECL MIA without an exogenous anodic coreactant, which can eliminate detrimental effects of multiplex coreactants and anodic ECL emission from CdTe NCs. The ICT within Zr-ADIP-HMT nanoparticles could shorten the electron transport path and reduce the complexity of radical intermediate transport. The ECL intensity from Zr-ADIP-HMT was 18.6-fold that from the mixture of H₄ADIP and HMT. In potential-resolved ECL MIA, two lung cancer biomarkers, carcinoembryonic antigen and neuron-specific enolase, were adopted as model analytes, with detection limits of 18 and 5.3 fg·mL^–1, respectively. The dual-ligand Zr-ADIP-HMT nanoparticles provide a proof of concept using ICT-based self-ECL luminophores for potential-resolved ECL MIAs with isolated coreactants.

更新日期：2023-06-23

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