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甲醇/二甲醚的选择性氧化转化

Selective oxidation conversion of methanol/dimethyl ether.

作者信息

Gao Xiujuan, Zhang Junfeng, Song Faen, Zhang Qingde, Han Yizhuo, Tan Yisheng

机构信息

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Science, Taiyuan 030001, China.

University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

Chem Commun (Camb). 2022 Apr 12;58(30):4687-4699. doi: 10.1039/d1cc07276e.

Abstract

As important platform compounds, methanol and dimethyl ether (DME) are vital bridges between the coal chemical, petrochemical and fine chemical industries. At present, the synthesis of methanol/DME has been industrialized, and the production capacity is much larger than the market demand. Therefore, the conversion of methanol/DME into more valuable chemicals is an important and significant topic. The synthesis of high value-added oxygenated chemicals and diesel oil additives from methanol/DME by an oxidation method has attracted substantial attention due to it being green and environmentally friendly and having good atom economy. In this feature article, we have summarized the recent advances in the synthesis of formaldehyde, methyl formate, dimethoxymethane, and polyoxymethylene dimethyl ethers, from the selective oxidation of methanol/DME, and further discussed the adsorption and activation of reactant molecules, selective cleavage of C-O, C-H or O-H bonds in methanol/DME molecules and the C-O chain growth in the target products. In the end, major challenges and future prospects are proposed from the viewpoint of catalyst design and application. It is expected that this feature article will provide theoretical guidance for the activation and cleavage of C-O, C-H, or O-H bonds in other small molecules of alcohol/ether as well as low-carbon alkanes, so as to synthesize high value-added chemicals.

摘要

甲醇和二甲醚(DME)作为重要的平台化合物,是煤化工、石油化工和精细化工行业之间至关重要的桥梁。目前,甲醇/二甲醚的合成已实现工业化,其产能远大于市场需求。因此,将甲醇/二甲醚转化为更具价值的化学品是一个重要且有意义的课题。通过氧化法由甲醇/二甲醚合成高附加值含氧化合物和柴油添加剂,因其绿色环保且具有良好的原子经济性而备受关注。在这篇专题文章中,我们总结了甲醇/二甲醚选择性氧化合成甲醛、甲酸甲酯、甲缩醛和聚甲醛二甲醚的研究进展,并进一步探讨了反应物分子的吸附与活化、甲醇/二甲醚分子中C - O、C - H或O - H键的选择性断裂以及目标产物中的C - O链增长。最后,从催化剂设计与应用的角度提出了主要挑战和未来展望。期望这篇专题文章能为醇/醚类其他小分子以及低碳烷烃中C - O、C - H或O - H键的活化与断裂提供理论指导,从而合成高附加值化学品。

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