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首页> 外文期刊>Electrochimica Acta >Charge transfer and SEIRAS studies of 1,4-benzoquinone functionalized mixed monothiol/dithiol self-assembled monolayers
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Charge transfer and SEIRAS studies of 1,4-benzoquinone functionalized mixed monothiol/dithiol self-assembled monolayers

机译：1,4-苯醌功能化的单硫醇/二硫醇混合自组装单分子膜的电荷转移和SEIRAS研究

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摘要

Although substantial information can be obtained from electrochemical measurements, much greater detail concerning molecular structure can be obtained by coupling such measurements with molecular spectroscopy. To this end, electrochemical and in situ surface enhanced infrared spectroscopy (SEIRAS) was performed to analyze 1,4-benzoquinone (BQ) terminated self-assembled monolayers. Monolayers were derived via the Michael addition of BQ to a pre-formed mixed monolayer composed of methyl and thiol terminated functionalities. This approach resulted in relatively robust but non-ideal redox-active monolayers. Spectroscopic and electrochemical measurements have allowed us to determine the pH dependence of both the apparent formal potential and the heterogeneous standard rate constant for proton coupled electron transfer (PCET) for this 2e~-/2H~+ redox system. While the former is in excellent agreement with predictions of step-wise PCET, the latter deviates from the expected kinetic response.
机译：尽管可以从电化学测量中获得大量信息，但是可以通过将这种测量与分子光谱学结合获得关于分子结构的更多细节。为此，进行了电化学和原位表面增强红外光谱（SEIRAS），以分析1,4-苯醌（BQ）终止的自组装单层。通过将BQ的迈克尔加成到由甲基和硫醇封端的官能团组成的预先形成的混合单层中，可以得出单层。这种方法导致了相对坚固但非理想的氧化还原活性单层。光谱和电化学测量使我们能够确定该2e〜-/ 2H〜+氧化还原系统的质子耦合电子转移（PCET）的表观形式电位和非均相标准速率常数的pH依赖性。前者与逐步PCET的预测非常吻合，而后者则偏离了预期的动力学响应。

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