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首页> 外文期刊>Electrocatalysis >Evaluating Activity for Hydrogen-Evolving Cobalt and Nickel Complexes at Elevated Pressures of Hydrogen and Carbon Monoxide
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Evaluating Activity for Hydrogen-Evolving Cobalt and Nickel Complexes at Elevated Pressures of Hydrogen and Carbon Monoxide

机译：在升高的氢气和一氧化碳压力下评估析氢钴和镍配合物的活性

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摘要

Molecular cobalt and nickel complexes are among the most promising homogeneous systems for electrocatalytic hydrogen evolution. However, there has been little exploration into the effect of gaseous co-additives such as CO and H-2, which may be present in operating hydrogen-evolving or carbon-dioxide reduction systems, on the performance of these molecular electrocatalysts. In this report, we investigate the electrocatalytic activity of six cobalt and nickel complexes supported by tetraazamacrocyclic or diazadiphosphacyclooctane ligands for the reduction of p-toluenesulfonic acid to hydrogen in acetonitrile under inert atmosphere and in the presence of CO and H-2. We present an elevated-pressure electrochemical apparatus capable of reaching CO and H-2 pressures of ca. 15-520 pounds per square inch (psia) (similar to 1-35 atm), and we use this apparatus to determine binding constants for CO addition for each catalyst and study the inhibition of the electrocatalysis as a function of CO and H-2 pressure. In the case of CO, the extent of catalytic inhibition is correlated to the binding constant, with the cobalt complexes showing a greater degree of catalyst inhibition compared to the nickel complexes. In the case of H-2, no complex showed appreciable electrocatalytic inhibition even at H-2 pressures of ca. 500 psia.
机译：分子钴和镍配合物是用于电催化制氢的最有希望的均相系统。然而，很少有人研究在操作的析氢或二氧化碳还原系统中可能存在的气态共添加剂（例如CO和H-2）对这些分子电催化剂的性能的影响。在本报告中，我们研究了四氮杂大环或二氮杂二磷环辛烷配体负载的六种钴和镍配合物的电催化活性，该反应在惰性气氛下以及在CO和H-2存在下，将对甲苯磺酸还原为乙腈中的氢。我们提出了一种高压电化学装置，能够达到大约1的CO和H-2压力。 15-520磅/平方英寸（psia）（与1-35 atm相似），我们使用此设备确定每种催化剂对CO加成的结合常数，并研究电催化与CO和H-2的关系压力。在CO的情况下，催化抑制的程度与结合常数相关，钴配合物显示出比镍配合物更大的催化剂抑制程度。在H-2的情况下，即使在大约H-2的压力下，也没有络合物显示出明显的电催化抑制作用。 500磅/平方英寸

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