A tunable LDI-MS platform assisted by metal-phenolic network-coated AuNPs for sensitive and customized detection of amino acids.

IF 5.6 1区化学 Q1 CHEMISTRY, ANALYTICAL Talanta Pub Date : 2025-01-01 Epub Date: 2024-09-21 DOI:10.1016/j.talanta.2024.126928

Tong Hu, Qi Sang, Dingyitai Liang, Wenjing Zhang, Yuning Wang, Kun Qian

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Abstract

This study introduces a novel approach for the sensitive and accurate detection of small molecule metabolites, employing metal-phenolic network (MPN) functionalized AuNPs as both adsorbent and matrix to enhance laser desorption/ionization mass spectrometry (LDI-MS) performance. The MPN comprising tannic acid (TA) and transition metal ions (Fe³⁺, Co²⁺, Ni²⁺, Cu²⁺, or Zn²⁺) was coated on the surface of AuNPs, forming metal-TA network-coated AuNPs (M-TA@AuNPs). The M-TA@AuNPs provided a tunable surface for specific interactions with analytes, displaying distinct enrichment efficacies for different amino acids, especially for Cu-TA@AuNPs exhibiting the highest affinity for histidine (His). Under the optimized condition, the proposed method enabled ultrasensitive detection of His, with good linearity (R² = 0.9627) in the low-concentration range (50 nM-1 μM) and a limit of detection (LOD) as low as 0.9 nM. Furthermore, the method was successfully applied to detect His from human urine samples, showcasing its practical applications in clinical diagnostics, particularly in the realm of amino acid-based targeted metabolomics.

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由金属酚网络包裹的 AuNPs 辅助的可调 LDI-MS 平台，用于灵敏和定制的氨基酸检测。

本研究采用金属酚网络（MPN）功能化 AuNPs 作为吸附剂和基质，提高了激光解吸电离质谱（LDI-MS）的性能，为灵敏准确地检测小分子代谢物提供了一种新方法。由单宁酸（TA）和过渡金属离子（Fe3+、Co2+、Ni2+、Cu2+或Zn2+）组成的MPN被包覆在AuNPs表面，形成金属-TA网络包覆的AuNPs（M-TA@AuNPs）。M-TA@AuNPs 提供了一个与分析物进行特异性相互作用的可调表面，对不同氨基酸具有不同的富集效果，尤其是 Cu-TA@AuNPs 对组氨酸（His）的亲和力最高。在优化的条件下，该方法可超灵敏地检测组氨酸，在低浓度（50 nM-1 μM）范围内线性关系良好（R2 = 0.9627），检出限（LOD）低至0.9 nM。此外，该方法还成功用于检测人体尿样中的His，展示了其在临床诊断中的实际应用，尤其是在基于氨基酸的靶向代谢组学领域。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Talanta 化学-分析化学

CiteScore

12.30

自引率

4.90%

发文量

861

审稿时长

29 days

期刊介绍： Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.