Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea.
ACS Nano. 2014 Mar 25;8(3):2848-56. doi: 10.1021/nn406657b. Epub 2014 Feb 24.
In this paper, we report the development of a versatile platform for a highly efficient and stable graphene oxide (GO)-based optical sensor that exhibits distinctive ratiometric color responses. To demonstrate the applicability of the platform, we fabricated a colorimetric, GO-based pH sensor that responds to a wide range of pH changes. Our sensing system is based on responsive polymer and quantum dot (QD) hybrids integrated on a single GO sheet (MQD-GO), with the GO providing an excellent signal-to-noise ratio and high dispersion stability in water. The photoluminescence emissions of the blue and orange color-emitting QDs (BQDs and OQDs) in MQD-GO can be controlled independently by different pH-responsive linkers of poly(acrylic acid) (PAA) (pKa=4.5) and poly(2-vinylpyridine) (P2VP) (pKa=3.0) that can tune the efficiencies of Förster resonance energy transfer from the BQDs to the GO and from the OQDs to the GO, respectively. As a result, the color of MQD-GO changes from orange to near-white to blue over a wide range of pH values. The detailed mechanism of the pH-dependent response of the MQD-GO sensor was elucidated by measurements of time-resolved fluorescence and dynamic light scattering. Furthermore, the MQD-GO sensor showed excellent reversibility and high dispersion stability in pure water, indicating that our system is an ideal platform for biological and environmental applications. Our colorimetric GO-based optical sensor can be expanded easily to various other multifunctional, GO-based sensors by using alternate stimuli-responsive polymers.
在本文中,我们报告了一种基于氧化石墨烯(GO)的多功能高效稳定光学传感器平台的开发,该平台具有独特的比率比色响应。为了展示该平台的适用性,我们制备了一种基于比色法的 GO 基 pH 传感器,该传感器对广泛的 pH 变化有响应。我们的传感系统基于响应性聚合物和量子点(QD)杂化物集成在单个 GO 片上(MQD-GO),GO 提供了在水中优异的信噪比和高分散稳定性。在 MQD-GO 中,蓝、橙色发光 QD(BQDs 和 OQDs)的光致发光发射可以通过不同的 pH 响应性聚(丙烯酸)(PAA)(pKa=4.5)和聚(2-乙烯基吡啶)(P2VP)(pKa=3.0)的链接来独立控制,这些链接可以分别调节 BQDs 到 GO 和 OQDs 到 GO 的Förster 共振能量转移效率。结果,MQD-GO 的颜色从橙色变为近白色再变为蓝色,覆盖了很宽的 pH 值范围。通过时间分辨荧光和动态光散射测量,阐明了 MQD-GO 传感器的 pH 依赖性响应的详细机制。此外,MQD-GO 传感器在纯水中表现出优异的可逆性和高分散稳定性,表明我们的系统是生物和环境应用的理想平台。通过使用其他刺激响应性聚合物,我们的基于比色法的 GO 光学传感器可以很容易地扩展到各种其他多功能 GO 基传感器。