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大多數(shù)化學發(fā)光（CL）底物表現(xiàn)出閃光型發(fā)光。因此，持久耐用的CL系統(tǒng)始終是基于CL的分析方法領(lǐng)域中的佼佼者。在這項工作中，我們構(gòu)建了Dox-ABEI嵌合磁性DNA水凝膠（MDH）作為新型的無蛋白酶持久CL反應系統(tǒng)。功能性MDH由于其對延遲共反應物擴散速率的阻滯作用，可將閃蒸型ABEI / H2O2 / CO2 +反應轉(zhuǎn)變?yōu)檩x光型CL體系，使CL反應逐漸發(fā)生。更重要的是，功能性MDH具有生物相容性和可控性的優(yōu)勢，可以進行精心設計以結(jié)合不同的生物傳感策略。隨后，我們建立了基于功能性MDH的長效CL免疫分析系統(tǒng)，用于d-二聚體和纖維蛋白降解產(chǎn)物（FDP）的超靈敏和高度特異性檢測。設計的CL免疫測定法可分別檢測低至53.7和31.6 fg / mL的d-二聚體和FDP，范圍從100 fg / mL到100 ng / mL的寬譜線，優(yōu)于以前報道的CL生物傳感策略。此外，得益于MDH的磁選和優(yōu)異的CL性能，該開發(fā)的免疫測定方法已成功應用于臨床樣品的檢測，與臨床參考技術(shù)密切相關(guān)。因此，該功能性MDH被證明是出色的持久CL系統(tǒng)和臨床生物分析應用的潛在技術(shù)平臺。

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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