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基于 MXene 纳米片的 N、S 共掺杂石墨烯量子点用于人血清中 3-硝基-L-酪氨酸的灵敏和选择性检测。

MXene nanosheet-derived N, S-codoped graphene quantum dots for ultrasensitive and selective detection of 3-nitro-l-tyrosine in human serum.

机构信息

Institute of Analytical and Environmental Sciences, National Tsing Hua University, 101 Section 2, Kuang-Fu Road, Hsinchu, 300044, Taiwan; Vinh Long University of Technology Education, 73 Nguyen Hue Street, Vinh Long City, Viet Nam.

Institute of Analytical and Environmental Sciences, National Tsing Hua University, 101 Section 2, Kuang-Fu Road, Hsinchu, 300044, Taiwan.

出版信息

Anal Chim Acta. 2024 Mar 1;1292:342237. doi: 10.1016/j.aca.2024.342237. Epub 2024 Jan 12.

Abstract

3-Nitro-l-tyrosine (3NT) is an oxidative stress metabolite associated with neurodegenerative diseases such as Parkinson's disease and rheumatoid arthritis. In this study, the N, S-co-doped graphene quantum dots (NSGQDs) derived from nitrogen-doped TiCT MXene nanosheet via the hydrothermal method in the presence of mercaptosuccinic acid was synthesized as an optical sensing probe to detect 3NT in human serum. Tetramethyl ammonium hydroxide, the nitrogen source and delamination agent, was used to prepare nitrogen-doped MXene nanosheets via one step at room temperature. The as-prepared NSGQDs are uniform with an average size of 1.2 ± 0.6 nm, and can be stable in aqueous solution for at least 90 d to serve as the fluorescence probe. The N atoms in N-MXene reduce the restacking and aggregation of MXene nanosheets, while the sulfur dopant in NSGQDs increases the quantum yield from 6.2 to 12.1 % as well as enhances the selectivity of 3NT over the other 12 interferences via coordination interaction with nitro group in 3NT. A linear range of 0.02-150 μM in PBS and 0.05-200 μM in human serum with a recovery of 97-108 % for 3NT detection is observed. Moreover, the limit of detection can be lowered to 4.2 and 7 nM in PBS and 1 × diluted human serum, respectively. Results obtained clearly indicate the potential application of the N-TiCT derived NSGQD for effective detection of 3NT, which can open a window for the synthesis of doped GQDs via 2D MXene materials for ultrasensitive and selective detection of other biometabolites and biomarkers of neurodegenerative diseases in biological fluids.

摘要

3-硝基-L-酪氨酸(3NT)是一种与神经退行性疾病(如帕金森病和类风湿关节炎)相关的氧化应激代谢物。在这项研究中,通过在巯基丁二酸存在下的水热法,从氮掺杂 TiCT MXene 纳米片制备了 N、S 共掺杂石墨烯量子点(NSGQDs),用作光学传感探针来检测人血清中的 3NT。四甲基氢氧化铵作为氮源和剥离剂,通过一步法在室温下制备氮掺杂 MXene 纳米片。所制备的 NSGQDs 具有均匀的尺寸,平均尺寸为 1.2 ± 0.6nm,并且可以在水溶液中至少稳定 90d 以用作荧光探针。N-MXene 中的 N 原子减少了 MXene 纳米片的堆积和聚集,而 NSGQDs 中的硫掺杂剂通过与 3NT 中的硝基基团的配位相互作用,将量子产率从 6.2%提高到 12.1%,并提高了对 3NT 与其他 12 种干扰物的选择性。在 PBS 中可以观察到 0.02-150μM 的线性范围,在人血清中可以观察到 0.05-200μM 的线性范围,3NT 的回收率为 97-108%。此外,在 PBS 和 1×稀释的人血清中,检测 3NT 的检出限可以分别降低至 4.2 和 7nM。结果清楚地表明,通过二维 MXene 材料合成掺杂 GQDs 可以有效地检测 3NT,为检测生物流体中其他神经退行性疾病的生物标志物和生物代谢物提供了新的思路。

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