A single atom cobalt anchored MXene bifunctional platform for rapid, label-free and high-throughput biomarker analysis and tissue imaging
A single atom cobalt anchored MXene bifunctional platform for rapid, label-free and high-throughput biomarker analysis and tissue imaging
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DOI：
10.1016/j.bios.2023.115903
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发表时间：
2023-12-03
影响因子：
12.6
通讯作者：
Ma，Chunxia
中科院分区：
文献类型：
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作者：
Liang，Weiqiang;Yan，Weining;Ma，Chunxia
在表面辅助激光解吸电离质谱（SALDI-MS）中，很少有单原子材料作为分析小分子的平台。本文中，制备了一种新型的单Co原子锚定的MXene（Co-N-Ti 3C 2），以首次实现增强的SALDI-MS和质谱成像（MSI）性能。采用简单的原位自组装方法制备了Co-N-Ti 3C 2薄膜，构建了高效的SALDI-MS平台。与传统的无机/有机基质相比，Co-N-Ti 3C 2薄膜具有上级的小分子检测性能，具有超高的灵敏度（阿莫尔限为100 μ L）、良好的重复性（CV <4%）、干净的背景和广泛的分析物覆盖范围，能够在几秒钟内对1 μL生物体液中的各种低浓度代谢物进行准确的定量分析。它的使用有效地增强了SALDI-MS检测各种小分子生物标志物，如氨基酸，琥珀酸，衣康酸，花生四烯酸，瓜氨酸，前列腺素E2，肌酐，尿酸，谷氨酰胺，D-甘露糖，胆固醇和肌醇在正离子模式。在线性浓度范围（0.25-10 mM）内成功测定了人体血糖水平。值得注意的是，Co-N-Ti 3C 2辅助SALDI-MSI能够在组织切片上以高分辨率研究小分子的空间分布，覆盖代谢组学的中心范围。此外，Co-N-Ti 3C 2平台揭示了一种区分骨关节炎（OA）和类风湿性关节炎（RA）组织的特定峰型。密度泛函理论研究表明，单个Co原子锚定在Ti 3C 2上，可以极大地增强代谢物的电离能力，导致高灵敏度和异质性的代谢物组覆盖。
Few of single-atom materials have been served as platform to analyze small molecules for surface assisted laser desorption/ionization mass spectrometry (SALDI-MS). Herein, a novel single Co atom-anchored MXene (Co–N–Ti3C2) is prepared to achieve enhanced SALDI-MS and mass spectrometry imaging (MSI) performance for the first time. The Co–N–Ti3C2films were prepared by a simple in situ self-assembly strategy to generate an efficient SALDI-MS platform. Compared to typical inorganic/organic matrices, Co–N–Ti3C2films exhibit superior performance in small molecules detection with ultra-high sensitivity (LOD at amol level), excellent repeatability (CV <4%), clean background and wide analyte coverage, enabling accurate quantitative analysis of various low-concentration metabolites from 1 μL biofluid in seconds. Its usage efficiently enhanced SALDI-MS detection of various small-molecule biomarkers such as amino acids, succinic acid, itaconic acid, arachidonic acid, citrulline, prostaglandin E2, creatinine, uric acid, glutamine, D-mannose, cholesterol and inositol in positive ion mode. The blood glucose level in humans was successfully determined from a linearity concentration range (0.25–10 mM). Notably, the Co–N–Ti3C2assisted SALDI-MSI enables study the spatial distribution of small molecules covering the range central to metabolomics at a high resolution on a tissue section. Furthermore, Co–N–Ti3C2platform revealed a specific peak profile that distinguishes osteoarthritis (OA) from rheumatoid arthritis (RA) tissue. Density functional theory theoretical investigation revealed that single Co atoms anchored on Ti3C2could highly enhanced the ionization ability of metabolites, resulting in high-sensitivity and heterogeneous metabolome coverage.