Structure Remodeling Strategy for Open-Cage NiFe@Fe-bis-PBA with Enhanced Peroxidase-like Activity To Monitor Tumor Markers,Analytical Chemistry

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Structure Remodeling Strategy for Open-Cage NiFe@Fe-bis-PBA with Enhanced Peroxidase-like Activity To Monitor Tumor Markers
Analytical Chemistry ( IF 6.7 ) Pub Date : 2024-09-13 , DOI: 10.1021/acs.analchem.4c02995
Ruixin Liu ₁ , Feng Shi ₁ , Haibing Zhu ₁ , Kai Liu ₁ , Zijun Lai ₁ , Yaoyao Li ₂ , Zhanjun Yang ₁ , Juan Li ₁

Affiliation

The inherent metal elements and structures of Prussian blue analogue (PBA) nanozymes have restricted their enzyme-mimicking activity. Therefore, the rational regulation of PBA nanozymes to improve their catalytic activity is highly desirable for biosensing applications. Herein, we propose a structure remodeling strategy to construct an open-cage Fe PBA-anchored NiFePBA (NiFe@Fe bis-PBA) nanozyme with significantly enhanced enzyme-mimicking activity. The formation process and mechanism for this bis-PBA nanozyme were studied in detail. Specifically, a cubic NiFePBA precursor was first synthesized and modified with polyvinylpyrrolidone (PVP). With the aid of hydrochloric acid, the added potassium ferricyanide was reduced by PVP and re-coordinated on the surface of NiFePBA to form the NiFe@Fe bis-PBA nanozyme with a special open-cage core–shell structure. The resultant NiFe@Fe bis-PBA nanozyme was further exploited to immobilize secondary antibodies, serving as a novel signal probe for developing highly sensitive electrochemical immunosensors for monitoring tumor markers. The constructed electrochemical immunosensor possesses a very wide linear range of 0.005–100 ng/mL and a low detection limit of 0.89 pg/mL for alpha-fetoprotein with high specificity and acceptable reproducibility and stability. This work offers a general and promising strategy for remodeling PBA nanozymes with a very favorable structure and metal element distribution, which enhances their enzyme-mimicking properties for applications in different fields.

中文翻译：

具有增强的过氧化物酶样活性的开笼式 NiFe@Fe-bis-PBA 的结构重塑策略，用于监测肿瘤标志物

普鲁士蓝类似物（PBA）纳米酶固有的金属元素和结构限制了其模拟酶活性。因此，合理调控PBA纳米酶以提高其催化活性对于生物传感应用来说是非常必要的。在此，我们提出了一种结构重塑策略来构建开笼式 Fe PBA 锚定 NiFePBA (NiFe@Fe bis-PBA) 纳米酶，其模拟酶活性显着增强。对这种双-PBA纳米酶的形成过程和机制进行了详细研究。具体来说，首先合成了立方体 NiFePBA 前驱体，并用聚乙烯吡咯烷酮 (PVP) 进行改性。在盐酸的帮助下，添加的铁氰化钾被PVP还原并在NiFePBA表面重新配位，形成具有特殊开笼核壳结构的NiFe@Fe bis-PBA纳米酶。所得的 NiFe@Fe bis-PBA 纳米酶被进一步用于固定二抗，作为一种新型信号探针，用于开发用于监测肿瘤标志物的高灵敏度电化学免疫传感器。构建的电化学免疫传感器对甲胎蛋白具有0.005-100 ng/mL的宽线性范围和0.89 pg/mL的低检测限，具有高特异性和可接受的重现性和稳定性。这项工作为重塑 PBA 纳米酶提供了一种通用且有前景的策略，使其具有非常有利的结构和金属元素分布，从而增强了其在不同领域的应用的模拟酶特性。

更新日期：2024-09-13

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