振动强耦合对葡萄糖氧化酶在电化学催化反应中的调控研究

Research on the Regulation of Glucose Oxidase in Electrochemical Catalysis under Vibrational Strong Coupling

摘要: 振动强耦合(Vibrational Strong Coupling, VSC)通过光–物质相互作用可以改变分子能级和反应势垒，以此调控多种生化反应。电化学对电极表面的电子转移过程具有较高的灵敏度，但将VSC与电化学结合以调控生物催化反应的相关研究仍然有限。本研究以葡萄糖氧化酶(Glucose Oxidase, GOD)在法布里珀罗(FP)腔内催化葡萄糖的氧化反应为模型，构建了电化学-FP腔体系，系统研究了FP腔与水的O-H伸缩振动(3409 cm⁻¹)耦合对该反应的影响。结果表明，通过调谐FP腔与水分子的耦合强度，GOD的催化率最高被抑制至原来的37% (抑制率达63%)，且在不同耦合强度下，GOD的催化率与水的O-H伸缩振动带密切相关。这项工作不仅揭示了VSC对生物电化学反应的调控作用，也表明电化学可用于实时监测FP腔内的反应过程，为VSC在生物电化学体系中的应用提供了新的实验证据。

Abstract: Vibrational Strong Coupling (VSC) can modulate molecular energy levels and reaction barriers through light-matter interactions, thereby regulating biochemical reactions. Although electrochemistry is highly sensitive to electron transfer at electrode interfaces, studies combining VSC with electrochemistry to control biocatalytic reactions remain limited. Here, glucose oxidation catalyzed by Glucose Oxidase (GOD) within a Fabry-Pérot (FP) cavity was used as a model system, and an electrochemical FP-cavity platform was established to investigate the effect of coupling between the FP cavity and the O-H stretching vibration of water (3409 cm⁻¹). By tuning the coupling strength, GOD catalytic activity was suppressed to as low as 37% of its original rate (maximum inhibition of 63%), and the catalytic rate showed a clear correlation with the water O-H stretching band under different coupling conditions. These findings reveal the regulatory effect of VSC on bioelectrochemical reactions and demonstrate that electrochemistry can be used for real-time monitoring of reactions within the FP cavity, providing new experimental evidence for the application of VSC in bioelectrochemical systems.