Department of Physical and Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario M1C 1A4, Canada.
Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada.
ACS Appl Mater Interfaces. 2023 Jun 14;15(23):27502-27514. doi: 10.1021/acsami.3c01600. Epub 2023 Jun 2.
In this proof-of-concept study, an ultralight graphene oxide aerogel (GOx-Aero) decorated with bimetallic palladium-iron nanoparticles (Pd-Fe) was synthesized and immobilized on a glassy carbon electrode (GCE) for electrochemical sensor applications. The main objective of this work was to develop a sensitive electrochemical sensor capable of simultaneously detecting eight biomolecules, including ascorbic acid (AA), dopamine (DA), uric acid (UA), 8-hydroxyguanine (8HG), guanine (G), adenine (A), thymine (T), and cytosine (C). To the best of our knowledge, this is the first time that an electrochemical sensor has been able to detect eight biomolecules simultaneously. The bimetallic GOx aerogel significantly enhanced the performance of the sensor by increasing the electroactive area, conductivity, and anodic peak current response. The sensor demonstrated sharp, well-defined, and continuous oxidation peaks for all eight analytes of interest and wide linear ranges of 5.0-1750, 0.25-100.0, 0.5-500.0, 0.5-375.0, 0.5-500.0, 0.5-500.0, 5.0-1500.0, and 5.0-1500.0 μM for AA, DA, UA, 8HG, G, A, T, and C, respectively. The prepared sensor also exhibited excellent stability, reproducibility, and sensitivity with a very low limit of detection (LOD) of 553.7, 1.8, 69.6, 43.2, 42.9, 72.3, 57.2, and 318.4 nM for AA, DA, UA, 8HG, G, A, T, and C, respectively. The Pd-Fe-GOx-Aero-GCE was also tested in various real samples such as artificial saliva, artificial cerebrospinal fluid (CSF), salmon sperm DNA, and genomic DNA from calf thymus, where it demonstrated good recovery values. Additionally, the novel developed sensor was used to monitor the interaction between the anticancer drug, cisplatin, which has well-described binding affinity with the G and A bases in DNA. Overall, Pd-Fe-GOx-Aero-GCE displayed an extremely promising platform not only for the simultaneous detection of eight biomolecules in complex biological matrices but also for DNA-drug interaction studies toward the development of electrochemical high-throughput drug screening assays, which is of great importance in the field.
在这项概念验证研究中,我们合成了一种负载双金属钯铁纳米粒子(Pd-Fe)的超轻氧化石墨烯气凝胶(GOx-Aero),并将其固定在玻碳电极(GCE)上,用于电化学传感器应用。本工作的主要目的是开发一种灵敏的电化学传感器,能够同时检测 8 种生物分子,包括抗坏血酸(AA)、多巴胺(DA)、尿酸(UA)、8-羟基鸟嘌呤(8HG)、鸟嘌呤(G)、腺嘌呤(A)、胸腺嘧啶(T)和胞嘧啶(C)。据我们所知,这是首次能够同时检测 8 种生物分子的电化学传感器。双金属 GOx 气凝胶通过增加电活性面积、电导率和阳极峰电流响应,显著提高了传感器的性能。该传感器对所有 8 种感兴趣的分析物都表现出尖锐、清晰和连续的氧化峰,并且具有宽的线性范围,分别为 5.0-1750、0.25-100.0、0.5-500.0、0.5-375.0、0.5-500.0、0.5-500.0、5.0-1500.0 和 5.0-1500.0 μM,用于 AA、DA、UA、8HG、G、A、T 和 C。制备的传感器还表现出出色的稳定性、重现性和灵敏度,检测限(LOD)非常低,分别为 553.7、1.8、69.6、43.2、42.9、72.3、57.2 和 318.4 nM,用于 AA、DA、UA、8HG、G、A、T 和 C。Pd-Fe-GOx-Aero-GCE 还在各种实际样品中进行了测试,例如人工唾液、人工脑脊液(CSF)、鲑鱼精 DNA 和小牛胸腺基因组 DNA,结果显示出良好的回收率。此外,该新型传感器还用于监测抗癌药物顺铂与 DNA 中 G 和 A 碱基之间的相互作用,顺铂与 G 和 A 碱基具有良好的结合亲和力。总的来说,Pd-Fe-GOx-Aero-GCE 不仅为在复杂生物基质中同时检测 8 种生物分子提供了一个极具前景的平台,还为 DNA-药物相互作用研究提供了一个平台,有助于开发电化学高通量药物筛选分析,这在该领域具有重要意义。