Oxidation of Methacrolein to Methacrylic Acid over Cu, P, Mo, V-Composites

IF 14.1 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Weihua Wang, Wenjie Xu, Nan Zhang, Mingming Chen, Jingqing Zhang, Hongxing Liu, Jianqiang Wang, Yongfeng Hu
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Abstract

The purpose of this study is to develop novel P-Mo-V heteropoly compound catalysts for the oxidation of methacrolein to methacrylic acid. The introduction of Cu, as a modifying element, was employed to enhance the catalytic performance. Experimental results show that the addition of Cu significantly improved the catalyst performance, increasing the conversion rate of methacrolein from 17.2% to 84.2%, while the yield of methacrylic acid was boosted from 5.5% to 51.7%. A series of characterization results showed that both P-Mo-V and Cu-P-Mo-V catalysts primarily exhibited the crystal phase of [PMo12O40]3−, with a small amount of [PMo11VO40]3− phase. However, the Cu-P-Mo-V catalyst exhibited much better oxidation–reduction ability compared to the P-Mo-V catalyst. Isolated Cu atoms were found to exist in a highly decentralized tetrahedral coordination structure, bridged by oxygen atoms within the heteropoly compound framework. The addition of Cu resulted in notable alterations in the modulation of the surface electronic structure, enhancement of oxidation–reduction ability, and optimization of the reaction pathway, thereby improving the overall catalytic activity of the catalyst. This study not only provides new insights into the modification of P-Mo-V heteropoly compound catalysts but also lays a foundation for understanding their catalytic mechanisms in organic synthesis reactions, demonstrating the potential of modifying elements in improving catalyst performance.

Abstract Image

甲基丙烯在Cu, P, Mo, v复合材料上氧化生成甲基丙烯酸
本研究的目的是开发新型的P-Mo-V杂多化合物催化剂,用于甲基丙烯醛氧化制甲基丙烯酸。引入Cu作为修饰元素,提高了催化剂的催化性能。实验结果表明,Cu的加入显著改善了催化剂的性能,甲基丙烯的转化率由17.2%提高到84.2%,甲基丙烯酸的收率由5.5%提高到51.7%。一系列表征结果表明,P-Mo-V和Cu-P-Mo-V催化剂主要表现为[PMo12O40]3−相,少量[PMo11VO40]3−相。Cu-P-Mo-V催化剂表现出比P-Mo-V催化剂更好的氧化还原能力。发现孤立的Cu原子以高度分散的四面体配位结构存在,在杂多化合物框架内由氧原子桥接。Cu的加入显著改变了催化剂的表面电子结构,增强了氧化还原能力,优化了反应途径,从而提高了催化剂的整体催化活性。本研究不仅为P-Mo-V杂多化合物催化剂的改性提供了新的见解,而且为了解其在有机合成反应中的催化机理奠定了基础,展示了修饰元素在提高催化剂性能方面的潜力。
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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