Enhanced Chemiluminescence under the Nanoconfinement of Covalent–Organic Frameworks and Its Application in Sensitive Detection of Cancer Biomarkers,Analytical Chemistry

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Enhanced Chemiluminescence under the Nanoconfinement of Covalent–Organic Frameworks and Its Application in Sensitive Detection of Cancer Biomarkers
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-05-11 , DOI: 10.1021/acs.analchem.3c00372
Aihua Lyu ₁ , Yisha Wang ₁ , Hua Cui ₁

Affiliation

Chemiluminescence (CL) with intensive emission has been pursued for decades. It is still challenging to find a new mechanism to enhance CL. In this work, confinement-enhanced CL was developed for the first time by the coembedding of N-(aminobutyl)-N-(ethylisoluminol) (ABEI) and Co²⁺ into gold nanoparticle-modified covalent–organic frameworks (COFs). For the consideration of improving the hydrophilicity of COFs and facilitating subsequent biological modification, gold nanoparticles were first reduced on the COF surface (Au-COF) in situ without other reducing reagents. By virtue of the abundant imine bond and π backbones, ABEI and Co²⁺ were embedded in Au-COF synergistically through π–π stacking and coordination. The confinement of ABEI and Co²⁺ into Au-COF brought an over 20-fold enhancement of CL intensity compared to that of adding them to a liquid phase, which benefitted from the three aspects of the confinement effect, including the molecular enrichment effect, the physical constraint effect, and the molecular preorganization effect. As proof of concept, a lipid–protein dual-recognition sandwich strategy based on this CL-functionalized COF was developed for the detection of breast cancer cell line-derived extracellular vesicles (EVs) with four orders of magnitude improvement in the detection limit compared to ELISA. The successful distinction of human epidermal growth factor receptor 2 (HER2)-positive patients from HER2-negative patients indicated the great application potential of the proposed bioassay in HER2-positive breast cancer diagnosis. This work proposed a novel enhancement mechanism for CL based on crystalline porous materials, which provides a new perspective for the development of CL-functionalized materials for biosensors and bioassays.

中文翻译：

共价有机骨架纳米限制下的增强化学发光及其在癌症生物标志物灵敏检测中的应用

几十年来，人们一直在追求具有强发射的化学发光 (CL)。找到一种新的机制来增强 CL 仍然具有挑战性。^{在这项工作中，通过将 N-(氨基丁基)-N-(乙基异鲁米诺) (ABEI) 和 Co 2+}共嵌入到金纳米颗粒修饰的共价有机框架 (COF) 中，首次开发了限制增强的 CL。出于提高 COFs 亲水性及便于后续生物修饰的考虑，金纳米粒子首先在 COFs 表面（Au-COF）原位还原，无需其他还原剂。凭借丰富的亚胺键和π主链，ABEI和Co ²⁺通过π-π堆积和配位协同嵌入Au-COF中。^{ABEI和Co 2+}的禁闭与将它们添加到液相中相比，Au-COF 中的发光强度提高了 20 多倍，这得益于限制效应的三个方面，包括分子富集效应、物理约束效应和分子预组织效应作为概念证明，开发了一种基于这种 CL 功能化 COF 的脂质-蛋白质双重识别夹心策略，用于检测乳腺癌细胞系衍生的细胞外囊泡 (EV)，与酶联免疫吸附试验。人类表皮生长因子受体 2 (HER2) 阳性患者与 HER2 阴性患者的成功区分表明所提出的生物测定在 HER2 阳性乳腺癌诊断中具有巨大的应用潜力。

更新日期：2023-05-11

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