College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, Hubei, P. R. China.
Anal Chem. 2022 Dec 27;94(51):17787-17794. doi: 10.1021/acs.analchem.2c03433. Epub 2022 Dec 15.
Gastric cancer is a malignant tumor, and its early diagnosis remains challenging due to the lack of simple and sensitive detection methods and specific biomarkers. In this work, to improve the detection reliability, we developed a dual-mode detection strategy for the detection of two biomarkers associated with it. First, an N- and S-doped carbon dots-N-rich porous carbon nanoenzyme (N/S-CDs@NC) was prepared by a two-step pyrolysis of thiourea-penetrated zinc-based zeolite imidazole framework. It was then combined with the 3,3',5,5'-tetramethylbenzidine-HO system for the colorimetric detection of d-amino acids (i.e., d-proline (d-Pro) and d-alanine (d-Ala)) in saliva, based on d-amino acid oxidase catalyzing d-amino acid oxidation to produce HO. In this way, the low detection limits (S/N = 3) of d-Pro and d-Ala were 0.14 and 0.35 μM, respectively. Furthermore, N/S-CDs@NC was combined with the luminol-HO electrochemiluminescence (ECL) system and magnetic immune accumulation/separation strategy to detect the carcinoembryonic antigen (CEA) in serum. The porous N/S-CDs@NC could facilitate participant contact, promote the generation of hydroxyl radical (OH), and electrostatically attract OH, thereby significantly amplifying the ECL signal of luminol and improving the signal stability. Thus, the detection mode showed considerable sensitivity and selectivity, with a low detection limit of 0.26 pg mL. The strategy proposed in this work can also be used for the detection of other disease markers by substituting the recognition elements, thus having good application potential.
胃癌是一种恶性肿瘤,由于缺乏简单而敏感的检测方法和特定的生物标志物,其早期诊断仍然具有挑战性。在这项工作中,为了提高检测可靠性,我们开发了一种用于检测两种与其相关的生物标志物的双模检测策略。首先,通过两步热解硫脲渗透的锌基金属有机骨架,制备了 N 和 S 掺杂的碳点-富氮多孔碳纳米酶(N/S-CDs@NC)。然后,它与 3,3',5,5'-四甲基联苯胺-HO 系统结合,用于唾液中 d-氨基酸(即 d-脯氨酸(d-Pro)和 d-丙氨酸(d-Ala))的比色检测,基于 d-氨基酸氧化酶催化 d-氨基酸氧化生成 HO。通过这种方式,d-Pro 和 d-Ala 的低检测限(S/N = 3)分别为 0.14 和 0.35 μM。此外,N/S-CDs@NC 与鲁米诺-HO 电化学发光(ECL)系统和磁性免疫富集/分离策略相结合,用于检测血清中的癌胚抗原(CEA)。多孔的 N/S-CDs@NC 可以促进参与者的接触,促进羟基自由基(OH)的生成,并静电吸引 OH,从而显著放大鲁米诺的 ECL 信号,提高信号稳定性。因此,该检测模式具有相当的灵敏度和选择性,检测限低至 0.26 pg mL。通过替换识别元件,本工作提出的策略也可用于检测其他疾病标志物,因此具有良好的应用潜力。