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首页> 外文期刊>ACS catalysis >Covalent Immobilization of (2,2 '-Bipyridyl) (Pentamethylcyclopentadienyl)-Rhodium Complex on a Porous Carbon Electrode for Efficient Electrocatalytic NADH Regeneration
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Covalent Immobilization of (2,2 '-Bipyridyl) (Pentamethylcyclopentadienyl)-Rhodium Complex on a Porous Carbon Electrode for Efficient Electrocatalytic NADH Regeneration

机译：在多孔碳电极上的（2,2'-BiPyridyl）（五甲基环戊二烯基）-Rhodium络合物的共价固定化，以有效电催化NADH再生

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摘要

Covalent bonding of (2,2'-bipyridyl) (pentamethylcyclopentadienyl)-rhodium complex at the surface of a carbon-based porous electrode was achieved by combining diazonium electrografting, Huisgen cycloaddition, and metal complexation. The immobilized catalyst was applied to electrochemical regeneration of the reduced form of nicotinamide adenine dinucleotide (NADH). The different steps of surface functionalization were characterized by X-ray photoelectron spectroscopy and electrochemistry. The Faradaic efficiency of NADH regeneration was 87%. The chemical bonding provided good stability in solution under convection over 14 days, which is much better than the simple adsorption of the Rh complex on the electrode surface. Finally, the system was tested in the presence of NAD-dependent dehydrogenases that were immobilized in a sol gel film on the top of the functionalized porous carbon electrode. A total turnover of 3790 and turnover frequency of 164 h(-1) was observed. Two enzymatic reactions were considered: D-fructose reduction to D-sorbitol catalyzed by D-sorbitol dehydrogenase and hydroxyacetone reduction to 1,2-propanediol with galactitol dehydrogenase. The electrocatalytic regeneration of 1 mM NADH by the immobilized rhodium species was kept after 90 h electrolysis in the conditions of electroenzymatic synthesis.
机译：通过组合重氮电解，Huisgen环加装饰和金属络合，实现（2,2'-双吡啶基）（五甲基环戊二烯基）-Rhodium复合物的共价键合。将固定化的催化剂应用于烟酰胺腺嘌呤二核苷酸（NADH）的减少形式的电化学再生。通过X射线光电子体光谱和电化学表征表面官能化的不同步骤。 NADH再生的游览效率为87％。化学键合在14天内的对流下的溶液中提供了良好的稳定性，这比电极表面上的RH复合物的简单吸附得多。最后，在依赖于官能化多孔碳电极顶部的溶胶凝胶膜中固定的NAD依赖性脱氢酶的存在下进行测试。观察到3790的总成交量和164小时（-1）的周转频率。考虑了两种酶促反应：D-脱水醇脱氢酶和羟基丙酮催化的D-山梨糖醇和羟基丙酮与半乳糖醇脱氢酶催化至1,2-丙二醇的D-脱水糖醇。在电酶合成条件下90小时电解后，将固定的铑物质的电催化再生保持在电酶合成条件下。

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