Coordination-Driven Templated Synthesis of Hierarchically Porous Zeolitic Imidazolate Frameworks for Cascade Enzyme Cycle Amplification Coupled Immunoassay,ACS Applied Materials & Interfaces

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Coordination-Driven Templated Synthesis of Hierarchically Porous Zeolitic Imidazolate Frameworks for Cascade Enzyme Cycle Amplification Coupled Immunoassay
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-07-23 , DOI: 10.1021/acsami.4c06788
Fan Xia ₁ , Jian Yang ₁ , Jingwen Chen ₁ , Ximeng Liu ₁ , Zhefan Ma ₁ , Jinlou Gu ₁

Affiliation

Although hierarchically porous zeolitic imidazolate frameworks (HPZIFs) not only inherit the intrinsic architectural and chemical stabilities of their microporous counterparts but also afford open space for the efficient mass diffusion of the macromolecules involved, their rational design and construction are still challenging. Herein, HPZIFs with tailorable pore sizes ranging from 18 to 54 nm were successfully fabricated by using a newly developed soft-template-directed strategy. Our success rooted in the fact that the screened PS₈₁–PVP₄₄–PEO₁₁₃ triblock copolymer could effectively coordinate with the metal precursor for the directed crystallization of ZIFs along surfactant assemblies. The advantages of continuous large pores and open structures in such HPZIFs were fully taken into account to serve as a bioreactor for the efficient immunoassay. The expanded large pores provided not only a significantly vast surface area to enhance the density of capture antibodies but also enough space for accommodating multiple conjugated biomolecules in one pore channel. In combination with a cascade enzyme cycle amplification strategy, a model biomarker of prostate-specific antigen (PSA) at the femtomolar level was checked with a limit of detection of 92 fM using the developed immunosensor. Specific screening on patients with prostate cancer or even benign prostatic hyperplasia was exemplified through accurately quantifying small changes of PSA concentration in clinical serum samples, prefiguring the great potential of the developed HPZIF-8 immunosensor platform for the early monitoring and diagnostics of diseases.

中文翻译：

用于级联酶循环扩增偶联免疫分析的分级多孔沸石咪唑酯框架的配位驱动模板化合成

尽管分级多孔沸石咪唑酯骨架（HPZIF）不仅继承了其微孔对应物的固有结构和化学稳定性，而且还为所涉及的大分子的有效质量扩散提供了开放空间，但其合理的设计和构造仍然具有挑战性。在此，通过使用新开发的软模板导向策略成功制造了孔径范围为 18 至 54 nm 的可定制 HPZIF。我们的成功源于这样一个事实：筛选的 PS ₈₁ –PVP ₄₄ –PEO ₁₁₃三嵌段共聚物可以有效地与金属前体配合，以沿着表面活性剂组装体定向结晶 ZIF。充分考虑了这种 HPZIF 的连续大孔和开放结构的优点，作为有效免疫测定的生物反应器。扩大的大孔不仅提供了极大的表面积以提高捕获抗体的密度，而且还提供了足够的空间在一个孔通道中容纳多个缀合的生物分子。结合级联酶循环扩增策略，使用开发的免疫传感器检查飞摩尔水平的前列腺特异性抗原（PSA）模型生物标志物，检测限为 92 fM。通过准确量化临床血清样本中PSA浓度的微小变化，举例说明了对前列腺癌甚至良性前列腺增生患者的特异性筛查，预示着所开发的HPZIF-8免疫传感器平台在疾病早期监测和诊断方面的巨大潜力。

更新日期：2024-07-23

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