Department of Electrical Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
ACS Appl Mater Interfaces. 2024 Nov 20;16(46):63142-63154. doi: 10.1021/acsami.4c11393. Epub 2024 Oct 29.
Despite the clinical data showing the importance of ascorbic acid (AA or vitamin C) in managing viral respiratory infections, biosensors for their simultaneous detection are lacking. To address this need, we developed a portable and wireless device for simultaneous detection of AA and SARS-CoV-2 virus by integrating commercial transistors with printed laser-induced graphene (LIG) as the extended gate. We studied the effect of laser printing pass number and showed that with two laser printing passes (2-pass LIG), the sensor sensitivity and limit of detection (LOD) for AA improved by a factor of 1.6 and 12.8, respectively. Using complementary characterization methods, we attribute the improved response to a balanced interplay of crystallinity, defect density, surface area, surface roughness, pore density and diameter, and mechanical integrity/stability. These factors enhance analyte transport, reduce noise/variability, and ensure consistent sensor performance, making 2-pass LIG the most effective material in this work. Our sensors exhibit promising performance for detecting AA with a selective response in the presence of common salivary interfering molecules, with sensitivity and LOD of 73.67 mV/dec and 54.04 nM in 1× phosphate buffered saline and 81.05 mV/dec and 78.34 nM in artificial saliva, respectively. We also showed that functionalization of the 2-pass LIG gate with S-protein antibody enables the detection of SARS-CoV-2 protein antigens with an ultralow LOD of 52 zg/mL─an improvement of more than 10-fold compared to 1-pass LIG─and 4 particles/mL for virion mimics with a selective response against influenza virus and multiple human coronavirus strains. With low signal drift/hysteresis and wireless capabilities, the developed device holds great potential for improving at-home monitoring and clinical decision-making.
尽管临床数据表明抗坏血酸(AA 或维生素 C)在管理病毒性呼吸道感染方面的重要性,但缺乏用于同时检测它们的生物传感器。为满足这一需求,我们通过将商用晶体管与印刷的激光诱导石墨烯(LIG)集成,开发了一种用于同时检测 AA 和 SARS-CoV-2 病毒的便携式无线设备,其中 LIG 作为扩展栅极。我们研究了激光打印遍数的影响,结果表明,通过两次激光打印(2 遍 LIG),传感器对 AA 的灵敏度和检测限(LOD)分别提高了 1.6 倍和 12.8 倍。通过互补的表征方法,我们将改善的响应归因于结晶度、缺陷密度、表面积、表面粗糙度、孔密度和直径以及机械完整性/稳定性的平衡相互作用。这些因素增强了分析物的传输,降低了噪声/变异性,并确保了传感器性能的一致性,使 2 遍 LIG 成为本工作中最有效的材料。我们的传感器在存在常见唾液干扰分子的情况下对 AA 具有选择性响应,在 1×磷酸盐缓冲盐水和人工唾液中的灵敏度和 LOD 分别为 73.67 mV/dec 和 54.04 nM、81.05 mV/dec 和 78.34 nM,表现出良好的性能。我们还表明,S 蛋白抗体对 2 遍 LIG 栅极的功能化可实现 SARS-CoV-2 蛋白抗原的检测,LOD 低至 52 zg/mL——比 1 遍 LIG 提高了 10 多倍——对流感病毒和多种人类冠状病毒株具有选择性响应的病毒模拟物的检测限为 4 个颗粒/mL。该开发的设备具有低信号漂移/滞后和无线功能,有望改善家庭监测和临床决策。