使用超颖表面驱动的表面增强红外吸收光谱改进电化学界面的原位表征
Improved in-situ characterization of electrochemical interfaces using metasurface-driven surface-enhanced infrared absorption spectroscopy
摘要：
电催化在实现向绿色能源过渡方面发挥着至关重要的作用，推动了从制氢到二氧化碳减排的研究方向。了解电化学反应对于提高其效率并弥合通往可持续零碳未来的差距至关重要。表面增强红外吸收光谱（SEIRAS）是一种合适的方法，用于研究这些过程，因为它可以监测化学特异性的反应机制。然而，它仍然难以检测电化学反应的许多相关方面，如短寿命的中间体。在这里，我们开发并实验实现了一个集成的纳米光子电化学SEIRAS平台，用于电化学实验过程中出现的分子信号痕迹的原位调查。具体来说，我们实现了一个铂纳米槽超颖表面具有强烈增强的电磁近场和光谱目标在弱振动弯曲模式的吸附CO在~2033 cm-1。至关重要的是，我们的铂纳米槽超颖表面提供高分子灵敏度。共振可以在中红外光谱的宽范围内调谐。与传统的非结构化铂层相比，我们的纳米光电化学平台将实验检测到的特征吸收信号大幅提高了27倍，从而能够检测到信号弱、转换快或表面浓度低的新物种。通过提供对催化反应的更深入了解，我们预计我们的纳米光子电化学平台将为电化学SEIRAS，表面增强拉曼光谱以及其他化学领域的反应研究（如光电催化）开辟令人兴奋的前景。
英文摘要：
Electrocatalysis plays a crucial role in realizing the transition towards green energy, driving research directions from hydrogen generation to carbon dioxide reduction. Understanding electrochemical reactions is crucial to improve their efficiency and to bridge the gap toward a sustainable zero-carbon future. Surface-enhanced infrared absorption spectroscopy (SEIRAS) is a suitable method for investigating these processes because it can monitor with chemical specificity the mechanisms of the reactions. However, it remains difficult to detect many relevant aspects of electrochemical reactions such as short-lived intermediates. Here, we develop and experimentally realize an integrated nanophotonic-electrochemical SEIRAS platform for the in situ investigation of molecular signal traces emerging during electrochemical experiments. Specifically, we implement a platinum nano-slot metasurface featuring strongly enhanced electromagnetic near fields and spectrally target it at the weak vibrational bending mode of adsorbed CO at ~2033 cm-1. Crucially, our platinum nano-slot metasurface provides high molecular sensitivity. The resonances can be tuned over a broad range in the mid-infrared spectrum. Compared to conventional unstructured platinum layers, our nanophotonic-electrochemical platform delivers a substantial improvement of the experimentally detected characteristic absorption signals by a factor of 27, enabling the detection of new species with weak signals, fast conversions, or low surface concentrations. By providing a deeper understanding of catalytic reactions, we anticipate our nanophotonic-electrochemical platform to open exciting perspectives for electrochemical SEIRAS, surface-enhanced Raman spectroscopy, and the study of reactions in other fields of chemistry such as photoelectrocatalysis.
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