College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, People's Republic of China.
State Key Laboratory of Medicinal Chemical Biology, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Research Center for Analytical Sciences, and College of Chemistry, Nankai University, Tianjin 300071, People's Republic of China.
Anal Chem. 2023 Mar 28;95(12):5443-5453. doi: 10.1021/acs.analchem.3c00449. Epub 2023 Mar 17.
The detection of hydrogen sulfide (HS), the third gas signaling molecule, is a promising strategy for identifying the occurrence of certain diseases. However, the conventional single- or dual-signal detection can introduce false-positive or false-negative results, which ultimately decreases the diagnostic accuracy. To address this limitation, we developed a luminescent, photothermal, and electrochemical triple-signal detection platform by optically trapping the synthetic highly doped upconversion coupled SiO microbeads coated with metal-organic frameworks H-UCNP-SiO@HKUST-1 (H-USH) to detect the concentration of HS. The H-USH was first synthesized and proved to have stable structure and excellent luminescent, photothermal, and electrochemical properties. Under 980 nm optical trapping and 808 nm irradiation, H-USH showed great detection linearity, a low limit of detection, and high specificity for HS quantification via triple-signal detection. Moreover, H-USH was captured by optical tweezers to realize quantitative detection of HS content in serum of acute pancreatitis and spontaneously hypertensive rats. Finally, by analyzing the receiver operating characteristic (ROC) curve, we concluded that triple-signal detection of HS was more accurate than single- or dual-signal detection, which overcame the problem of false-negative/positive results in the detection of HS in actual serum samples.
硫化氢（HS）的检测作为第三种气体信号分子，是识别某些疾病发生的一种很有前途的策略。然而，传统的单信号或双信号检测可能会引入假阳性或假阴性结果，从而降低诊断的准确性。为了解决这一局限性，我们通过光学捕获合成的高度掺杂上转换耦合 SiO 微球来开发了一种发光、光热和电化学三重信号检测平台，该微球涂有金属有机骨架 H-UCNP-SiO@HKUST-1（H-USH）以检测 HS 的浓度。首先合成了 H-USH，并证明其具有稳定的结构和优异的发光、光热和电化学性能。在 980nm 光捕获和 808nm 照射下，H-USH 通过三重信号检测表现出出色的检测线性度、低检测限和对 HS 定量检测的高特异性。此外，H-USH 被光学镊子捕获，以实现急性胰腺炎和自发性高血压大鼠血清中 HS 含量的定量检测。最后，通过分析接收器工作特征（ROC）曲线，我们得出结论，HS 的三重信号检测比单信号或双信号检测更准确，克服了实际血清样本中 HS 检测中假阴性/阳性结果的问题。
