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Effect on the Ligand of Triruthenium Unit for Hydrogen Evolution Reaction

机译：三钌单元配位体对析氢反应的影响

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At present, various energy problems occur on the earth. In order to solve the problems utilization of hydrogen is a candidate. Because hydrogen is a clean and highly efficient energy that does not produce sulfur oxides and nitrogen oxides and is attracting attention as a substitute for primary energy such as petroleum and natural gas. In this study, we focused on the ruthenium cluster unit (1-mer) forming a cyclic structure having three ruthenium ions in a mixed-valence state. Here, we examined a catalytic function of hydrogen evolution reaction (HER) at the 1-mer modified highly oriented pyrolytic graphite (HOPG) electrode. In addition, we have studied effects of alcohol as ligands for 1-mer. Cyclic voltammetry (CV) and linear sweep voltammetry (LSV) were used for electrochemical measurements. HOPG was modified by drop casting of 0.5 μM 1-mer dichloromethane or methanol solution and used as a working electrode. A Ag/AgCl (KCl sat.) or a reversible hydrogen electrode (RHE) was used as a reference electrode, and a platinum plate was used as a counter electrode. LSV and CV were carried out in 0.1 M HClO_4 in the presence of various alcohols such as methanol and ethanol. Figure 1 shows the LSVs of 0.1 M HClO_4 at the 1-mer modified HOPG. The surface concentration of 1-mer was cocurated to be 18 nmol cm~(-2). At the 1-mer modified HOPG electrode, the starting potential of HER was slightly shifted to positive as compared with that of bare HOPG electrode. This means that the 1-mer modified HOPG has a little catalytic activity for HER. On the other hand, addition of alcohol to the system changes drastically the catalytic activity of the HER. Onset potential of HER was shifted to positive by the addition of alcohol. Comparing the current densities in the presence of each alcohol at -0.80 V, the HER current was influenced by the kinds of alcohol. Especially, when methanol was added to the system, the current density of 0.02 A cm~(-2) at - 0.80 V. Although the reason why the catalytic current for HER depends on the type of alcohol is not clear, it may be considered that the THF ligands of 1-mer are substituted by the alcohol used. We have been are studying the effect of surface concentration and nanoscale structure of 1-mer, and the anion of the electrolyte.
机译：目前，地球上出现了各种各样的能源问题。为了解决这些问题，氢的利用是一个候选方案。因为氢是一种清洁高效的能源，不产生硫氧化物和氮氧化物，并且作为石油和天然气等一次能源的替代品而受到关注。在这项研究中，我们重点研究了形成环状结构的钌团簇单元（1-mer），该环状结构具有三个混合价态的钌离子。在这里，我们研究了1-聚体修饰的高取向热解石墨（HOPG）电极上析氢反应（HER）的催化功能。此外，我们还研究了乙醇作为1-聚体配体的作用。循环伏安法（CV）和线性扫描伏安法（LSV）用于电化学测量。用0.5μm1-二氯甲烷或甲醇溶液滴注改性HOPG，并将其用作工作电极。Ag/AgCl（KCl-sat.）或可逆氢电极（RHE）用作参比电极，铂板用作对电极。LSV和CV在0.1 M HClO_4中，在甲醇和乙醇等各种醇的存在下进行。图1显示了0.1 M HClO_4在单体改性HOPG中的LSV。1-聚体的表面浓度被确定为18nmol cm-2。在1-聚体修饰的HOPG电极上，HER的起始电位与裸HOPG电极相比略微偏移为正。这意味着1-聚体修饰的HOPG对她有一点催化活性。另一方面，向系统中添加酒精会极大地改变HER的催化活性。通过添加酒精，她的发病潜能变为阳性。比较在-0.80 V下存在每种酒精时的电流密度，HER电流受酒精种类的影响。特别是，当向系统中添加甲醇时，在-0.80 V下的电流密度为0.02 A cm-2。尽管对她的催化电流取决于乙醇类型的原因尚不清楚，但可以认为1-聚体的THF配体被所用的乙醇取代。我们一直在研究1-聚体的表面浓度和纳米结构以及电解质阴离子的影响。

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