用于羧酸和 N,N-二烷基甲酰胺高效直接氧化氨化的 CCF@GO 纳米催化剂的单锅合成与优化

IF 3.7 2区 化学 Q2 CHEMISTRY, APPLIED Applied Organometallic Chemistry Pub Date : 2024-08-26 DOI:10.1002/aoc.7728
Mahesh A. Pawar, Akhil V. Nakhate, Priti V. Ugemuge, Samidha S. Kadu, Pradip V. Tekade
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引用次数: 0

摘要

本研究提出了一种使用 CuCoFe2O4@GO(CCF@GO)通过羧酸和 N,N-二烷基甲酰胺的直接偶联合成酰胺键(-CONH-)的高效催化方案。通过改变铜和钴的比例(1:1、1:3 和 3:1),采用单锅溶热法合成了 CCF@GO 纳米催化剂。利用苯甲酸和二甲基甲酰胺(DMF)的模型反应进行催化剂筛选后发现,1:1 比例的 CCF@GO 催化剂具有极佳的催化效率,对酰胺的形成具有很高的转化率(98%)。CCF@GO 催化剂催化效率的提高可归因于活性铜和钴物种在具有高比表面积的氧化石墨烯载体上的均匀分布。通过改变温度、溶剂、催化剂负载和氧化剂等参数对反应进行了优化。利用 XRD、FTIR、XPS、SEM、EDX 图谱和 TEM 等多种分析技术对制备的催化剂进行了表征。此外,这种异质纳米催化剂还表现出了使用外部磁铁的可回收性,可重复使用多达五次,而催化性能仅略有下降。
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Single-Pot Synthesis and Optimization of CCF@GO Nanocatalyst for Efficient Direct Oxidative Amidation of Carboxylic Acids and N,N-Dialkylformamides

In this study, an efficient catalytic protocol using CuCoFe2O4@GO (CCF@GO) for the synthesis of amide bond (−CONH−) via direct coupling of carboxylic acids and N,N-dialkylformamides is presented. The CCF@GO nanocatalyst has been synthesized via a single-pot solvothermal method, by changing the proportions of copper and cobalt (1:1, 1:3, and 3:1). Catalyst screening, employing a model reaction with benzoic acid and dimethylformamide (DMF), revealed that the 1:1 proportion of CCF@GO catalyst exhibited excellent efficiency, achieving a high conversion (98%) towards amide formation. The enhanced catalytic efficiency observed in CCF@GO catalysts can be ascribed to the uniform distribution of active copper and cobalt species on the graphene oxide support, which possesses a high surface area. Optimization of the reaction was conducted by varying parameters such as temperature, solvent, catalyst loading, and oxidant. The prepared catalyst was characterized using various analytical techniques including XRD, FTIR, XPS, SEM, EDX mapping, and TEM. Furthermore, this heterogeneous nanocatalyst demonstrated recoverability using an external magnet and reused up to five times with just a modest loss of catalytic performance.

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来源期刊
Applied Organometallic Chemistry
Applied Organometallic Chemistry 化学-无机化学与核化学
CiteScore
7.80
自引率
10.30%
发文量
408
审稿时长
2.2 months
期刊介绍: All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.
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