Preparation of CuOx@PC derived from Cu-BTC with polyvinylpyrrolidone and the catalytic performance for oxidative carbonylation of methanol to dimethyl carbonate

Li, Wenjie; Gao, Shanlin; Lai, Chunbo; Lin, Huibo; Wang, Xinyu; Xiao, Wanjing; Li, Xinling; Xu, Chenghua; Deng, Zhiyong

doi:10.1016/j.matchemphys.2023.128759

Cited by 2 publications

(1 citation statement)

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“…CuCl and CuCl 2 are known as effective catalysts for oxidative carbonylation of methanol. , However, the poor solubility of CuCl in methanol made the industrial reaction system a slurry liquid and chloride loss led to equipment corrosion and catalyst deactivation. , Thus, many researchers had tried to add, e.g., amines and pyridines as promoters or immobilized copper salts on supports in order to avoid these problems . Nitrogen-containing ligands such as N -methylimidazole (NMI) can coordinate with copper ions to form copper–organic complex catalysts, promoting the dissolution and increasing the catalytic activity of cuprous chloride, which significantly reduces the corrosion of equipment .…”

Section: Introductionmentioning

confidence: 99%

Mechanistic Investigation of Oxidative Methanol Carbonylation with Mixed Cu(I)/Cu(II)–N-Methylimidazole Catalysts

Li,

Wang,

Liu

et al. 2024

Ind. Eng. Chem. Res.

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Copper complex catalysts exhibit excellent activity for the oxidative carbonylation of methanol to produce dimethyl carbonate (DMC). However, the reaction mechanism over Cu(I) or Cu(II) complex catalysts is not fully understood. In this study, homogeneous CuCl/CuCl 2 −NMI-m/n (N = N-methylimidazole; m/n = molar ratio of Cu(I) and Cu(II)) catalysts with organic ligand coordination are designed for oxidative carbonylation. The optimized CuCl/CuCl 2 −NMI-0.3/0.7 catalyst showed a TOF as high as 3.4 h −1 and a DMC selectivity of 67.2% based on oxygen, which were superior to those of CuCl−NMI or CuCl 2 −NMI. Our experiments suggested that the high activity and selectivity were assigned to the synergistic effect between Cu(I) and Cu(II), in which Cu(I) and Cu(II) are mainly responsible for the rapid generation of copper carbonyl and copper methoxy intermediates, respectively. This synergistic effect not only enhances the reaction activity but also ensures high DMC selectivity.

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