大多数化学发光（CL）底物表现出闪光型发光。因此，持久耐用的CL系统始终是基于CL的分析方法领域中的佼佼者。在这项工作中，我们构建了Dox-ABEI嵌合磁性DNA水凝胶（MDH）作为新型的无蛋白酶持久CL反应系统。功能性MDH由于其对延迟共反应物扩散速率的阻滞作用，可将闪蒸型ABEI / H2O2 / CO2 +反应转变为辉光型CL体系，使CL反应逐渐发生。更重要的是，功能性MDH具有生物相容性和可控性的优势，可以进行精心设计以结合不同的生物传感策略。随后，我们建立了基于功能性MDH的长效CL免疫分析系统，用于d-二聚体和纤维蛋白降解产物（FDP）的超灵敏和高度特异性检测。设计的CL免疫测定法可分别检测低至53.7和31.6 fg / mL的d-二聚体和FDP，范围从100 fg / mL到100 ng / mL的宽谱线，优于以前报道的CL生物传感策略。此外，得益于MDH的磁选和优异的CL性能，该开发的免疫测定方法已成功应用于临床样品的检测，与临床参考技术密切相关。因此，该功能性MDH被证明是出色的持久CL系统和临床生物分析应用的潜在技术平台。

Novel Protease-Free Long-Lasting Chemiluminescence System Based on the Dox-ABEI Chimeric Magnetic DNA Hydrogel for Ultrasensitive Immunoassay
Haiping Wu, Min Zhao, Jia Li, Xiaoyan Zhou, Tiantian Yang, Dezhang Zhao, Ping Liu, Huangxian Ju, Wei Cheng*, and Shijia Ding*
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 42, 47270–47277

Most of chemiluminescence (CL) substrates exhibit the flash-type light emission. Therefore, the long-lasting CL system is always the crown in the field of CL-based analysis methodology. In this work, we constructed a Dox-ABEI chimeric magnetic DNA hydrogel (MDH) as a novel protease-free long-lasting CL reaction system. The functional MDH can transform flash-type ABEI/H2O2/CO2+ reaction into a glow-type CL system because of its block effect on delaying the diffusion rate of co-reactants, making the CL reaction gradually occur. More importantly, the functional MDH possessed the advantages of biocompatibility and controllability and could be well-designed to incorporate different biosensing strategies. Subsequently, we established a functional MDH-based long-lasting CL immunoassay system for ultrasensitive and highly specific detection of d-dimer and fibrin degradation products (FDPs). The designed CL immunoassay can detect d-dimer and FDP down to 53.7 and 31.6 fg/mL, respectively, with a wide line ranging from 100 fg/mL to 100 ng/mL, which was superior to the previously reported CL biosensing strategies. Moreover, benefiting from the magnetic separation of MDH and excellent CL performance, the developed immunoassaying method was successfully applied in the detection of clinical samples, which showed a close correlation with clinical reference technology. Thus, this functional MDH proved to be an excellent long-lasting CL system and a potential technical platform for clinical bioanalysis applications.

https://pubs.acs.org/doi/abs/10.1021/acsami.0c14188

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