Liu Yaoran, Wu Zilong, Kollipara Pavana Siddhartha, Montellano Richard, Sharma Kumar, Zheng Yuebing
Department of Electrical and Computer Engineering, The University of Texas at Austin, Austin, Texas 78712, United States.
Walker Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712, United States.
ACS Nano. 2021 Apr 27;15(4):6448-6456. doi: 10.1021/acsnano.0c08822. Epub 2021 Mar 24.
Homochirality is necessary for normal biochemical processes in humans. Abnormal amounts of chiral molecules in biofluids have been found in patients with diabetes. However, the detailed analysis of diabetes-related abnormal chirality in biofluids and its potential use for clinical applications have been hindered by the difficulty in detecting and monitoring the chiral changes in biofluids, due to their low molar mass and trace concentrations. Herein, we demonstrate the label-free detection of chiral molecules using only 10 μL with 10-fold enhancement in sensitivity compared with traditional plasmonic chiral metamaterials. The ultrahigh sensitivity and low sample consumption were enabled by microbubble-induced rapid accumulation of biomolecules on plasmonic chiral sensors. We have applied our technique on mouse and human urine samples, uncovering the previously undetectable diabetes-induced abnormal dextrorotatory shift in chirality of urine metabolites. Furthermore, the accumulation-assisted plasmonic chiral sensing achieved a diagnostic accuracy of 84% on clinical urine samples from human patients. With the ultrahigh sensitivity, ultralow sample consumption, and fast response, our technique will benefit diabetes research and could be developed as point-of-care devices for first-line noninvasive screening and prognosis of prediabetes or diabetes and its complications.
同手性对于人类正常的生化过程是必要的。在糖尿病患者的生物流体中发现了异常数量的手性分子。然而，由于生物流体中手性变化的检测和监测存在困难，因其摩尔质量低且浓度痕量，生物流体中与糖尿病相关的异常手性及其在临床应用中的潜在用途的详细分析受到了阻碍。在此，我们展示了仅使用10 μL就能对手性分子进行无标记检测，与传统的等离子体手性超材料相比，灵敏度提高了10倍。微泡诱导生物分子在等离子体手性传感器上快速积累，实现了超高灵敏度和低样品消耗。我们已将我们的技术应用于小鼠和人类尿液样本，发现了尿液代谢物手性中先前无法检测到的糖尿病诱导的异常右旋转变。此外，积累辅助的等离子体手性传感在人类患者的临床尿液样本上实现了84%的诊断准确率。凭借超高灵敏度、超低样品消耗和快速响应，我们的技术将有益于糖尿病研究，并可开发为用于糖尿病前期或糖尿病及其并发症的一线无创筛查和预后的即时检测设备。
