Chandio Imamdin, Jiao Qisen, Li Ruiqi, Ai Yongjian, Liang Qionglin
MOE Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology, Department of Chemistry, Laboratory of Flexible Electronics Technology, Center for Synthetic and Systems Biology, Tsinghua University, Beijing 100084, P. R. China.
TUS-Pharmaceutical Group Co., Ltd., Hengyang 421200, Hunan, P. R. China.
ACS Appl Mater Interfaces. 2025 Jul 9;17(27):38960-38970. doi: 10.1021/acsami.5c08094. Epub 2025 Jun 28.
The development of biofunctional electrochemical aptasensors represents an emerging frontier in diagnostic technology, yet achieving precise and ultrasensitive detection of inflammatory bowel disease (IBD) biomarkers for early stage diagnosis remains a critical challenge. To overcome this, we engineered a novel material-based electrochemical aptasensor by using amino acid-functionalized high-entropy alloy nanosheets (HEANSs@AAs) for calprotectin (CP) detection. The fabricated HEANSs@AAs demonstrate remarkable electrochemical performance through their multielemental composition and mesoporous architecture, featuring abundant active sites enriched with several functional groups, which improve the surface chemistry of the composite for efficient immobilization of NH-aptamer. The HEANSs@AAs-based platform enables dual signal amplification through accelerated electron transfer kinetics and improved surface reactivity. The developed aptasensor demonstrates an ultrawide dynamic range (5 pg mL to 100 ng mL) with a limit of detection (LOD) of 2.02 pg mL (/ = 3). Significantly, the aptasensor exhibits 5.32% signal retention after 8 days storage at 4 °C and demonstrates an outstanding relative standard deviation (RSD) of 1.92%, revealing remarkable stability and reproducibility. The fabricated sensor revealed acceptable recovery rates in human serum samples between 96.6 and 97.6%, with inter-assay RSD below 2.7%, confirming its efficiency for clinical use. This work establishes a robust platform for early IBD diagnosis through precise CP quantification and introduces a versatile strategy for developing high-performance biosensors based on entropy-stabilized nanomaterials, thereby advancing multiplex biomarker detection in point-of-care diagnostic applications.
生物功能化电化学适体传感器的发展代表了诊断技术的一个新兴前沿领域，然而，实现对炎症性肠病（IBD）生物标志物的精确和超灵敏检测以进行早期诊断仍然是一项严峻挑战。为了克服这一挑战，我们通过使用氨基酸功能化的高熵合金纳米片（HEANSs@AAs）构建了一种新型的基于材料的电化学适体传感器，用于检测钙卫蛋白（CP）。所制备的HEANSs@AAs通过其多元素组成和介孔结构展现出卓越的电化学性能，其具有富含多个官能团的丰富活性位点，这改善了复合材料的表面化学性质，以实现NH-适配体的有效固定。基于HEANSs@AAs的平台通过加速电子转移动力学和改善表面反应性实现双信号放大。所开发的适体传感器表现出超宽的动态范围（5 pg/mL至100 ng/mL），检测限（LOD）为2.02 pg/mL（n = 3）。值得注意的是，该适体传感器在4℃储存8天后信号保留率为5.32%，并表现出1.92%的出色相对标准偏差（RSD），显示出卓越的稳定性和重现性。所制备的传感器在人血清样品中的回收率在96.6%至97.6%之间，批间RSD低于2.7%，证实了其临床应用的有效性。这项工作通过精确的CP定量建立了一个用于IBD早期诊断的强大平台，并引入了一种基于熵稳定纳米材料开发高性能生物传感器的通用策略，从而推动了即时诊断应用中的多重生物标志物检测。
