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Immobilization-Enabled Proton Reduction Catalysis by a Di-iron Hydrogenase Mimic

机译：固定化的质子还原催化双铁氢化酶模拟。

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We have long been interested in the influence of surface immobilization on the electrochemical integrity of redox-active moieties [1-5]. Our studies have shown that, if the electroactive group itself is directly chemisorbed on (coordinated to) the electrode surface, profound alterations result in both the thermodynamics and kinetics of the electron transfer processes; the oxidative chemisorption of the iodide anion (to zerovalent iodine atoms) or the hydroquinone molecule (to benzoquinone) are prototypical examples. The changes are more subtle and less dramatic if the electroactive site is only a pendant moiety tethered to the surface via an anchor group; mercapto hydroquinone bound exclusively via the-SH group is a well-known specimen. We recently extended our investigations to include enzyme-inspired molecular electrocatalysts in which the multinuclear reactive site may require a certain entatic state to carry out its catalytic function; the anticipation is that the motion-restricted surface-tethered species would suffer diminished catalytic activity. The results are described in this brief communication.
机译：我们长期以来对表面固定化对氧化还原活性部分的电化学完整性的影响感兴趣[1-5]。我们的研究表明，如果电活性基团本身直接化学吸附在电极表面上（与电极表面协调），则深刻的变化会导致电子转移过程的热力学和动力学变化。碘阴离子（至零价碘原子）或氢醌分子（至苯醌）的氧化化学吸附就是典型的例子。如果电活性位仅仅是通过锚定基团束缚在表面上的侧基部分，则变化将更加微妙，并且不那么引人注目。仅通过-SH基团结合的巯基对苯二酚是众所周知的样品。最近，我们将研究范围扩大到包括酶激发的分子电催化剂，其中多核反应位点可能需要一定的焓状态才能发挥其催化功能。预期运动受限的表面束缚物质将遭受催化活性的降低。在此简短的通讯中描述了结果。

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