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基于吡唑啉酮的草酰胺金属配合物插层到钠蒙脱石中用于以过氧化氢为氧化剂的苯酚催化液相氧化反应。

Intercalation of pyrazolone-based oxalamide metal complexes into Na-montmorillonite for catalytic liquid-phase oxidation of phenol using HO.

作者信息

Uzan Serhat, Başaran Eyüp

机构信息

Food Analysis Application and Research Center (BÜGAM), Batman University, Batman, Turkiye.

Department of Chemistry and Chemical Processing Technologies, Vocational School of Technical Sciences, Batman University, Batman, Turkiye.

出版信息

Turk J Chem. 2023 Oct 10;47(6):1497-1507. doi: 10.55730/1300-0527.3630. eCollection 2023.

DOI:10.55730/1300-0527.3630
PMID:38544712
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10965178/
Abstract

The intercalation of pyrazolone-based oxalamide metal complexes into Na-montmorillonite (Na-MMT) for catalytic liquid-phase oxidation of phenol using HO was undertaken by a flexible ligand method using metal ions including Mn(II), Zn(II), and Sn(II). First, the metal ions were exchanged with the sodium ions of Na-MMT, and then these metal ions were complexed with a new pyrazolone-based oxalamide ligand. The intercalated metal complexes were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, elemental analysis, and thermogravimetric analysis. Phenol was successfully oxidized by heterogeneous catalysts based on Mn(II), Zn(II), and Sn(II) pyrazolone-based oxalamide complexes intercalated into Na-MMT. These heterogeneous catalysts catalyze the liquid-phase oxidation of phenol using HO to catechol as the major product and hydroquinone and benzoquinone as the minor products. The Mn(II) and Zn(II) complexes intercalated into Na-MMT showed better activity than the Sn(II) complex intercalated into Na-MMT and the reaction without the catalyst. It has been shown that some metal ion complexes intercalated into Na-MMT are active catalysts for liquid-phase oxidation of phenol with hydrogen peroxide.

摘要

采用柔性配体法，利用包括Mn(II)、Zn(II)和Sn(II)在内的金属离子，将基于吡唑啉酮的草酰胺金属配合物插入钠蒙脱石(Na-MMT)中，用于以过氧化氢为氧化剂的苯酚催化液相氧化反应。首先，金属离子与Na-MMT中的钠离子进行交换，然后这些金属离子与一种新型的基于吡唑啉酮的草酰胺配体形成配合物。通过傅里叶变换红外光谱、X射线衍射、扫描电子显微镜、能量色散X射线光谱、元素分析和热重分析对插层金属配合物进行了表征。基于插入Na-MMT中的Mn(II)、Zn(II)和Sn(II)吡唑啉酮基草酰胺配合物的多相催化剂成功地将苯酚氧化。这些多相催化剂以过氧化氢为氧化剂，将苯酚液相氧化为主要产物邻苯二酚，对苯二酚和苯醌为次要产物。插入Na-MMT中的Mn(II)和Zn(II)配合物比插入Na-MMT中的Sn(II)配合物以及无催化剂的反应表现出更好的活性。研究表明，一些插入Na-MMT中的金属离子配合物是用过氧化氢进行苯酚液相氧化的活性催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/cee457676a45/tjc-47-06-1497f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/b8236ebf90d5/tjc-47-06-1497f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/322bdb27c37e/tjc-47-06-1497f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/da655487e4cf/tjc-47-06-1497f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/ddb6afd0dff8/tjc-47-06-1497f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/cc307229fb13/tjc-47-06-1497f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/7b8bf4050d6f/tjc-47-06-1497f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/1541626e7994/tjc-47-06-1497f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/cee457676a45/tjc-47-06-1497f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/b8236ebf90d5/tjc-47-06-1497f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/322bdb27c37e/tjc-47-06-1497f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/da655487e4cf/tjc-47-06-1497f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/ddb6afd0dff8/tjc-47-06-1497f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/cc307229fb13/tjc-47-06-1497f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/7b8bf4050d6f/tjc-47-06-1497f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/1541626e7994/tjc-47-06-1497f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e8b/10965178/cee457676a45/tjc-47-06-1497f8.jpg

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本文引用的文献

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Direct Hydroxylation of Benzene with Hydrogen Peroxide Using Fe Complexes Encapsulated into Mesoporous Y-Type Zeolite.介孔 Y 型沸石封装的铁配合物催化苯直接氧化生成过氧化氢。
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