含有非无害二酰胺基/双(膦)钳配体的镍、钯和铂配合物对 2-氨基乙醇的电催化自由基降解作用

IF 1.1 4区 物理与天体物理 Q4 PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
Ilya K. Mikhailov, Zufar N. Gafurov, Alexey A. Kagilev, Il’yas F. Sakhapov, Vladimir I. Morozov, Gumar R. Ganeev, Khasan R. Khayarov, Vasilisa A. Kulikova, Vladislava A. Kirkina, Evgenii I. Gutsul, Elena S. Shubina, Natalia V. Belkova, Oleg G. Sinyashin, Dmitry G. Yakhvarov
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引用次数: 0

摘要

使用循环伏安法研究了通式为 (PNP)MCl (PNP 为双(2-二异丙基膦-4-甲基苯基)酰胺;M = 镍、钯和铂)的 PNP 锌螯合物在 2-氨基乙醇(MEA,一种难降解污染物)氧化降解过程中的电催化活性。络合物符合氧化还原介质或催化剂的典型要求。它们在电化学氧化过程中会产生氨基自由基,这些自由基的未配对电子被定位在配体上。我们使用 ESR 和 NMR 光谱方法研究了这些氨基自由基配合物与 MEA 的相互作用机理。在模型铂衍生物的溶液中加入 MEA 后,氨基自由基复合物的 ESR 信号消失,而 31P{1H} NMR 光谱则显示出氨基自由基复合物的中性再生。NMR 光谱则显示出中性 (PNP)MCl 的再生。研究发现,钯衍生物是该系列中最有效的催化剂,其 Icat/Ip 值为 6.7。通过控制电位电解,我们确定了催化过程的主要产物,并提出了整个过程的机理。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Electrocatalytic Radical Degradation of 2-Aminoethanol by Nickel, Palladium and Platinum Complexes Bearing Non-Innocent Diarylamido/bis(Phosphine) Pincer Ligand

Electrocatalytic Radical Degradation of 2-Aminoethanol by Nickel, Palladium and Platinum Complexes Bearing Non-Innocent Diarylamido/bis(Phosphine) Pincer Ligand

Electrocatalytic Radical Degradation of 2-Aminoethanol by Nickel, Palladium and Platinum Complexes Bearing Non-Innocent Diarylamido/bis(Phosphine) Pincer Ligand

The electrocatalytic activity of PNP pincer complexes with general formula (PNP)MCl (PNP is bis(2-diisopropylphosphino-4-methylphenyl)amide; M = nickel, palladium and platinum) in the oxidative 2-aminoethanol (MEA, a recalcitrant pollutant) degradation process was studied using cyclic voltammetry method. Complexes fulfil the requirements typically expected of a redox mediator or catalyst. Their electrochemical oxidation yields the aminyl radical species which unpaired electron is localized on the ligand. The mechanism of interaction of these aminyl radical complexes with MEA was studied using ESR- and NMR-spectroscopy methods. The addition of MEA to the solution of model platinum derivative leads to the disappearance of the ESR signal responsible for the aminyl radical complex, whereas the 31P{1H} NMR spectrum revealed the regeneration of neutral (PNP)MCl. Palladium derivative was found to be the most effective catalyst of the series with an Icat/Ip value of 6.7. Controlled potential electrolysis has allowed us to identify the main products of the catalytic process and to propose the mechanism of the overall process.

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来源期刊
Applied Magnetic Resonance
Applied Magnetic Resonance 物理-光谱学
CiteScore
1.90
自引率
10.00%
发文量
59
审稿时长
2.3 months
期刊介绍: Applied Magnetic Resonance provides an international forum for the application of magnetic resonance in physics, chemistry, biology, medicine, geochemistry, ecology, engineering, and related fields. The contents include articles with a strong emphasis on new applications, and on new experimental methods. Additional features include book reviews and Letters to the Editor.
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