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首页> 外文期刊>Catalysis science & technology >Evaluating the role of acidic, basic, and polar amino acids and dipeptides on a molecular electrocatalyst for H-2 oxidation
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Evaluating the role of acidic, basic, and polar amino acids and dipeptides on a molecular electrocatalyst for H-2 oxidation

机译：评估酸性的作用、基本和极性的氨基酸和二肽分子electrocatalyst为氢氧化

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摘要

Amino acids and peptides have been shown to have a significant influence on the H-2 production and oxidation reactivity of Ni((P2N2R')-N-R)(2), where (P2N2R')-N-R = 1,5-diaza-3,7-diphosphacyclooctane, R is either phenyl (Ph) or cyclohexyl (Cy), and R' is either an amino acid or peptide. Most recently, the Ni((P2N2aminoacid)-N-CY)(2) complexes (CyAA) have shown enhanced H-2 oxidation rates, water solubility, and in the case of arginine (CyArg) and phenylalanine (CyPhe), electrocatalytic reversibility. Both the backbone-COOH and side chain interactions were shown to be critical to catalytic performance. Here we further investigate the roles of the outer coordination sphere by evaluating amino acids with acidic, basic, and hydrophilic side chains, as well as dipeptides which combine multiple successful features from previous complexes. Six new complexes were prepared, three containing single amino acids: aspartic acid (CyAsp), lysine (CyLys), and serine (CySer) and three containing dipeptides: glycine-phenylalanine (Cy(GlyPhe)), phenylalanine-glycine (Cy(PheGly)), and aspartic acid-phenylananine (Cy(AspPhe)). The resulting catalytic performance demonstrates that complexes need both interactions between side chain and -COOH groups for fast, efficient catalysis. The fastest of all of the catalysts, Cy(AspPhe), had both of these features, while the other dipeptide complexes with an amide replacing the -COOH were both slower; however, the amide group was demonstrated to participate in the proton pathway when side chain interactions are present to position it. Both the hydrophilic and basic side chains, notably lacking in side chain interactions, significantly increased the overpotential, with only modest increases in TOF. Of all of the complexes, only CyAsp was electro-catalytically reversible at room temperature, and only in water, the first of these complexes to demonstrate room temperature aqueous electrocatalytic reversibility for the H-2/H+ transformation. These results continue to provide and solidify design rules for controlling reactivity and efficiency of Ni(P2N2)(2) complexes with the outer coordination sphere.
机译：氨基酸和肽已被证明有一个2生产和显著的影响氧化镍的反应((P2N2R -N-R) (2),(P2N2R) -N-R =1、5-diaza-3 7-diphosphacyclooctane, R(Ph)或环己基苯(Cy)和R”一种氨基酸或肽。Ni ((P2N2aminoacid) -N-CY)(2)复合物(CyAA)显示增强的2氧化率、水的溶解度,精氨酸(CyArg)和苯丙氨酸(CyPhe), electrocatalytic可逆性。链相互作用被证明是至关重要的催化性能。调查外部协调的角色通过评估范围与酸性氨基酸,基本的,亲水侧链,以及二肽结合多个成功从先前的复合物功能。包含单一复合物被准备,三氨基酸:天冬氨酸(CyAsp),赖氨酸(CyLys)和丝氨酸(半胱氨酸)和三个包含二肽:glycine-phenylalanine (Cy (GlyPhe)),phenylalanine-glycine (Cy (PheGly))和天冬氨酸的acid-phenylananine (Cy (AspPhe))。催化性能表明,复合物侧链之间的相互作用和需要羧基组快速、高效催化。最快的催化剂,Cy (AspPhe)这两个特性,而另一个二肽复合物的酰胺取代羧基慢;证明了质子参与途径当侧链相互作用存在位置。链,尤其是缺乏侧链交互,大大增加了过电压,只有TOF的小幅增加。所有的复合物中,只有CyAspelectro-catalytically可逆在房间温度,只有在水里,第一的这些复合物来演示室温水electrocatalytic可逆性的h2 / H +转换。提供控制和巩固设计规则反应性和效率的倪(P2N2) (2)复合物与外部协调球体。

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