Spectroelectrochemical Network Measurements for Redox Bioelectronics,Chemistry of Materials

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Spectroelectrochemical Network Measurements for Redox Bioelectronics
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-01-17 , DOI: 10.1021/acs.chemmater.2c02707
Zhiling Zhao _{1,

2} , Eunkyoung Kim _{1,

2} , Dana Motabar _{1,

2,

3} , William E. Bentley _{1,

2,

3} , Gregory F. Payne _{1,

2}

Affiliation

Redox bioelectronics enlists electrochemical methods to connect to biology through biology’s native redox modality. The activities of this redox modality involve the exchange of electrons through redox reactions, and often, individual redox reactions are embedded within larger redox-reaction networks. Here, we examined electrodes coated with redox-active but non-conducting catechol-containing hydrogels that are emerging as important materials in redox-based bioelectronics. Previous studies have shown that electron “flow” through these catechol hydrogels involves redox reactions, and in some cases, catechol’s redox-state switching can be observed by orthogonal electrical and optical measurements. Here, we extend analysis by increasing the dimensionality of dynamic optical measurements from a single wavelength to a broader spectrum and adapt a minimal deterministic network model to reveal the intrinsic structure of this additional data. This increased dimensionality enhances our capabilities for detecting and interpreting discriminating signals, and we demonstrate these capabilities by comparing the response characteristics of conducting versus redox-active hydrogels and redox networks with different topologies. We discuss the importance of increasing measurement dimensionality to enhance both data-driven and theory-guided approaches for information processing in redox-based bioelectronics.

中文翻译：

氧化还原生物电子学的光谱电化学网络测量

氧化还原生物电子学采用电化学方法通过生物学的天然氧化还原方式与生物学联系起来。这种氧化还原模式的活动涉及通过氧化还原反应交换电子，并且通常，单个氧化还原反应嵌入更大的氧化还原反应网络中。在这里，我们检查了涂有氧化还原活性但不导电的含儿茶酚水凝胶的电极，这些水凝胶正在成为基于氧化还原的生物电子学中的重要材料。先前的研究表明，通过这些儿茶酚水凝胶的电子“流动”涉及氧化还原反应，在某些情况下，可以通过正交电学和光学测量来观察儿茶酚的氧化还原态转换。这里，我们通过将动态光学测量的维数从单个波长增加到更宽的光谱来扩展分析，并采用最小的确定性网络模型来揭示这些额外数据的内在结构。这种增加的维度增强了我们检测和解释区分信号的能力，我们通过比较导电与氧化还原活性水凝胶和具有不同拓扑结构的氧化还原网络的响应特性来证明这些能力。我们讨论了增加测量维数以增强基于氧化还原的生物电子学中信息处理的数据驱动和理论指导方法的重要性。这种增加的维度增强了我们检测和解释区分信号的能力，我们通过比较导电与氧化还原活性水凝胶和具有不同拓扑结构的氧化还原网络的响应特性来证明这些能力。我们讨论了增加测量维数以增强基于氧化还原的生物电子学中信息处理的数据驱动和理论指导方法的重要性。这种增加的维度增强了我们检测和解释区分信号的能力，我们通过比较导电与氧化还原活性水凝胶和具有不同拓扑结构的氧化还原网络的响应特性来证明这些能力。我们讨论了增加测量维数以增强基于氧化还原的生物电子学中信息处理的数据驱动和理论指导方法的重要性。

更新日期：2023-01-17

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