Ji Tiantian, Li Yige, Jiang Mingzhe, Cheng Yingying, Ren Haoyi, Li Hongling, Hong Chenglin
School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi 832003, PR China.
School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi 832003, PR China.
Bioelectrochemistry. 2026 Feb;167:109073. doi: 10.1016/j.bioelechem.2025.109073. Epub 2025 Aug 5.
The early and sensitive detection of cancer, a malignant disease posing significant threats to human health, is of strategic importance for disease prevention and control. This study employed 1,3,6,8-tetra(4-carboxyphenyl)pyrene (HTBAPy), a fluorophore exhibiting aggregation-caused quenching (ACQ), to construct a zinc-based metal-organic framework (Zn-TBAPy) serving as an energy donor platform. Polydopamine-coated ZIF-67 (ZIF-67@PDA) was employed as the energy acceptor to construct an electrochemiluminescence (ECL) immunosensor for sensitive carcinoembryonic antigen (CEA) detection. The advantages of ECL immunosensor are primarily manifested in the following three aspects: (1) Zn-TBAPy not only mitigates ACQ caused by polycyclic aromatic hydrocarbon π-π stacking but also enhances chromophore loading capacity and specific surface area. Relative to aggregate systems, the Zn-TBAPy exhibits a 2.5-fold enhancement in ECL signal intensity. (2) ZIF-67@PDA exhibits favorable broad-spectrum absorption characteristics and excellent quenching efficiency; as well as demonstrates superior biocompatibility for immunosensor construction. (3) The immunosensor was constructed through an electrochemiluminescence resonance energy transfer (ECL-RET) mechanism, yielding markedly improved sensitivity; the developed sensor demonstrated a linear detection range from100 fg·mL to 80 ng·mLwith LOD) of 0.275 pg·mL. In conclusion, this study provides a valuable research strategy for the construction of immunosensors based on novel luminophore materials.
癌症作为一种对人类健康构成重大威胁的恶性疾病，其早期和灵敏检测对于疾病预防和控制具有战略重要性。本研究采用1,3,6,8-四(4-羧基苯基)芘(HTBAPy)，一种具有聚集诱导猝灭(ACQ)特性的荧光团，构建了一个作为能量供体平台的锌基金属有机框架(Zn-TBAPy)。采用聚多巴胺包覆的ZIF-67(ZIF-67@PDA)作为能量受体，构建了一种用于灵敏检测癌胚抗原(CEA)的电化学发光(ECL)免疫传感器。ECL免疫传感器的优势主要体现在以下三个方面：(1)Zn-TBAPy不仅减轻了多环芳烃π-π堆积引起的ACQ，还提高了发色团负载能力和比表面积。相对于聚集体系，Zn-TBAPy的ECL信号强度提高了2.5倍。(2)ZIF-67@PDA具有良好的广谱吸收特性和优异的猝灭效率；并且在免疫传感器构建方面表现出卓越的生物相容性。(3)该免疫传感器通过电化学发光共振能量转移(ECL-RET)机制构建，灵敏度显著提高；所开发的传感器线性检测范围为100 fg·mL至80 ng·mL，检测限(LOD)为0.275 pg·mL。总之，本研究为基于新型发光体材料构建免疫传感器提供了一种有价值的研究策略。
