Department of Chemistry and Center of Excellence for Innovation in Chemistry, Faculty of Science, Ubon Ratchathani University, Ubon Ratchathani, 34190, Thailand.
Graphene and Printed Electronics for Dual-Use Applications Research Division (GPERD), National Science and Technology Development Agency (NSTDA), Pathum Thani, 12120, Thailand.
Talanta. 2023 Sep 1;262:124695. doi: 10.1016/j.talanta.2023.124695. Epub 2023 May 20.
We developed a novel, compact, three-dimensional electrochemical paper-based analytical device (3D-ePAD) for patulin (PT) determination. The selective and sensitive PT-imprinted Origami 3D-ePAD was constructed based on a graphene screen-printed electrode modified with manganese-zinc sulfide quantum dots coated with patulin imprinted polymer (Mn-ZnS QDs@PT-MIP/GSPE). The Mn-ZnS QDs@PT-MIP was synthesized using 2-oxindole as the template, methacrylic acid (MAA) as a monomer, N,N'-(1,2-dihydroxyethylene) bis (acrylamide) (DHEBA) as cross-linker and 2,2'-azobis (2-methylpropionitrile) (AIBN) as initiator, respectively. The Origami 3D-ePAD was designed with hydrophobic barrier layers formed on filter paper to provide three-dimensional circular reservoirs and assembled electrodes. The synthesized Mn-ZnS QDs@PT-MIP was quickly loaded on the electrode surface by mixing with graphene ink and then screen-printing on the paper. The PT-imprinted sensor provides the greatest enhancement in redox response and electrocatalytic activity, which we attributed to synergetic effects. This arose from an excellent electrocatalytic activity and good electrical conductivity of Mn-ZnS QDs@PT-MIP, which improved electron transfer between PT and the electrode surface. Under the optimized DPV conditions, a well-defined PT oxidation peak appears at +0.15 V (vs Ag/AgCl) using 0.1 M of phosphate buffer (pH 6.5) containing 5 mM KFe(CN) as the supporting electrolyte. Our developed PT imprinted Origami 3D-ePAD revealed excellent linear dynamic ranges of 0.001-25 μM, with a detection limit of 0.2 nM. Detection performance indicated that our Origami 3D-ePAD possesses outstanding detection performance from fruits and CRM in terms of high accuracy (%Error for inter-day is 1.11%) and precision (%RSD less than 4.1%). Therefore, the proposed method is well-suited as an alternative platform for ready-to-use sensors in food safety. The imprinted Origami 3D-ePAD is an excellent disposable device with a simple, cost-effective, and fast analysis, and it is ready to use for determining patulin in actual samples.
我们开发了一种新颖的、紧凑的、三维电化学纸质分析装置（3D-ePAD），用于测定棒曲霉素（PT）。基于石墨烯丝网印刷电极修饰的具有锰锌硫化量子点的选择性和灵敏的 PT 印迹折纸 3D-ePAD 被构建，所述锰锌硫化量子点涂覆有棒曲霉素印迹聚合物（Mn-ZnS QDs@PT-MIP/GSPE）。使用 2-氧吲哚作为模板，甲基丙烯酸（MAA）作为单体，N，N'-(1,2-二羟基乙烯）双（丙烯酰胺）（DHEBA）作为交联剂，2,2'-偶氮二（2-甲基丙腈）（AIBN）作为引发剂，分别合成 Mn-ZnS QDs@PT-MIP。通过将 Mn-ZnS QDs@PT-MIP 与石墨烯油墨混合并随后在纸上丝网印刷，将折纸 3D-ePAD 设计为在滤纸上形成疏水性阻挡层，以提供三维圆形储液器和组装电极。合成的 Mn-ZnS QDs@PT-MIP 通过混合并随后在纸上丝网印刷，快速加载到电极表面上。PT 印迹传感器提供了最大的氧化还原响应和电催化活性增强，我们认为这是协同作用的结果。这是由于 Mn-ZnS QDs@PT-MIP 的极好的电催化活性和良好的导电性，改善了 PT 与电极表面之间的电子转移。在优化的 DPV 条件下，在含有 5 mM KFe(CN)的 0.1 M 磷酸盐缓冲液（pH 6.5）中，使用+0.15 V（相对于 Ag/AgCl）出现了明确的 PT 氧化峰。作为支持电解质。我们开发的 PT 印迹折纸 3D-ePAD 显示出优异的线性动态范围为 0.001-25 μM，检测限为 0.2 nM。检测性能表明，我们的折纸 3D-ePAD 具有出色的检测性能，从水果和 CRM 中获得了高精度（日内%误差为 1.11%）和精密度（%RSD 小于 4.1%）。因此，该方法非常适合作为食品安全中即用型传感器的替代平台。印迹折纸 3D-ePAD 是一种出色的一次性设备，具有简单、经济高效和快速分析的特点，可随时用于实际样品中棒曲霉素的测定。
