Pyrene-Appended Boronic Acids on Graphene Foam Electrodes Provide Quantum Capacitance-Based Molecular Sensors for Lactate
Pyrene-Appended Boronic Acids on Graphene Foam Electrodes Provide Quantum Capacitance-Based Molecular Sensors for Lactate
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DOI：
10.1021/acssensors.4c00027
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发表时间：
2024-03-06
期刊：
影响因子：
8.9
通讯作者：
Marken，Frank
中科院分区：
文献类型：
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作者：
Wikeley，Simon M.;Przybylowski，Jakub;Marken，Frank
分子识别和传感可以耦合到石墨烯泡沫表面的界面电容变化，与双层效应相关，并耦合到增强的量子电容。3D石墨烯泡沫薄膜电极（gi - sens，厚度约40 μm，粗糙度系数约100）浸泡在水性缓冲介质中，在吸附基于芘附加硼酸（这里是4-硼-1-（芘-2-甲基）吡啶-1-溴化ium，简称T1）的带电分子受体后，电化学电容出现数量级的跳跃。这个附在芘上的吡啶硼酸受体在这里被用作乳酸的分子受体。在乳酸存在和pH为4.0时（pH优化后），电化学电容（通过阻抗谱测定）再次翻倍。乳酸结合以希利安结合常数表达（乳酸在缓冲液中= 75 mol - 1dm3, α = 0.8；乳酸在人工汗液中= 460 mol - 1dm3, α = 0.8；乳酸在人血清中= 340 mol - 1dm3, α = 0.65）。结果表明，该分子探针对LoD = 1.3、1.4和1.8 mM的乳酸分别在水溶液缓冲介质（pH 4.0）、人工汗液（调节至pH 4.7）和人血清（pH调节至4.0）中具有选择性响应。从双层结构和量子电容变化的角度讨论了芘附加硼酸的作用。在未来，这种新型分子电容传感器可以为更广泛的分析物和复杂的环境提供选择性无酶分析，而无需分析物消耗。
Molecular recognition and sensing can be coupled to interfacial capacitance changes on graphene foam surfaces linked to double layer effects and coupled to enhanced quantum capacitance. 3D graphene foam film electrodes (Gii-Sens; thickness approximately 40 μm; roughness factor approximately 100) immersed in aqueous buffer media exhibit an order of magnitude jump in electrochemical capacitance upon adsorption of a charged molecular receptor based on pyrene-appended boronic acids (here, 4-borono-1-(pyren-2-ylmethyl)pyridin-1-ium bromide, or abbreviated T1). This pyrene-appended pyridinium boronic acid receptor is employed here as a molecular receptor for lactate. In the presence of lactate and at pH 4.0 (after pH optimization), the electrochemical capacitance (determined by impedance spectroscopy) doubles again. Lactic acid binding is expressed with a Hillian binding constant (Klactate= 75 mol–1dm3and α = 0.8 in aqueous buffer,Klactate= 460 mol–1dm3and α = 0.8 in artificial sweat, andKlactate= 340 mol–1dm3and α = 0.65 in human serum). The result is a selective molecular probe response for lactic acid with LoD = 1.3, 1.4, and 1.8 mM in aqueous buffer media (pH 4.0), in artificial sweat (adjusted to pH 4.7), and in human serum (pH adjusted to 4.0), respectively. The role of the pyrene-appended boronic acid is discussed based on the double layer structure and quantum capacitance changes. In the future, this new type of molecular capacitance sensor could provide selective enzyme-free analysis without analyte consumption for a wider range of analytes and complex environments.