Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst

doi:10.1016/j.cjche.2018.02.018

Chinese Journal of Chemical Engineering ›› 2018, Vol. 26 ›› Issue (5): 1059-1063.DOI: 10.1016/j.cjche.2018.02.018

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst

Dong-Ho Lee^1,2, Jiin You¹, Je-Min Woo¹, Jung Yoon Seo¹, Young Cheol Park¹, Jong-Seop Lee¹, Hyunuk Kim³, Jong-Ho Moon¹, Seung Bin Park²

1 Greenhouse Gas Laboratory, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 34129, Korea;
2 Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Korea;
3 Energy Material Laboratory, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 34129, Korea

收稿日期:2017-10-19 修回日期:2018-01-19 出版日期:2018-05-28 发布日期:2018-06-29
通讯作者: Jong-Ho Moon,E-mail addresses:moon_jongho@kier.re.kr;Seung Bin Park,E-mail addresses:SeungBinPark@kaist.ac.kr

Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst

Dong-Ho Lee^1,2, Jiin You¹, Je-Min Woo¹, Jung Yoon Seo¹, Young Cheol Park¹, Jong-Seop Lee¹, Hyunuk Kim³, Jong-Ho Moon¹, Seung Bin Park²

1 Greenhouse Gas Laboratory, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 34129, Korea;
2 Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Korea;
3 Energy Material Laboratory, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 34129, Korea

Received:2017-10-19 Revised:2018-01-19 Online:2018-05-28 Published:2018-06-29
Contact: Jong-Ho Moon,E-mail addresses:moon_jongho@kier.re.kr;Seung Bin Park,E-mail addresses:SeungBinPark@kaist.ac.kr

摘要/Abstract

摘要： The influence of the dehydration by metal oxides on the synthesis of dimethyl carbonate (DMC) via oxidative carbonylation of methanol was studied. A Cu/Y-zeolite catalyst was prepared by the ion exchange method from CuCl₂·2H₂O and the commercial NH₄-form of the Y type zeolite. The catalyst was characterized by X-ray fluorescence (XRF), N2 adsorption (BET method), X-ray diffraction (XRD), and temperature-programmed desorption of ammonia (NH₃-TPD) to evaluate its Cu and Cl content, surface area, structure, and acidity. Reaction tests were carried out using an autoclave (batch reactor) for 18 h at 403 K and 5.5 MPa (2CH₃OH + 1/2O₂ + CO ? (CH₃O)₂CO + H₂O). The influence of various dehydrating agents (ZnO, MgO, and CaO) was examined with the aim of increasing the methanol conversion (X_MeOH, MeOH conversion). The MeOH conversion increased upon addition of metal oxides in the order CaO >> MgO > ZnO, with the DMC selectivity (S_DMC) following the order MgO > CaO > ZnO. The catalysts and dehydrating agents were characterized before and after the oxidative carbonylation of methanol by thermogravimetric and differential thermogravimetric (TG/DTG), and XRD to confirm that the dehydration reaction occurred via the metal oxide (MO + H₂O → M(OH)₂). The MeOH conversion increased from 8.7% to 14.6% and DMC selectivity increased from 39.0% to 53.1%, when using the dehydrating agent CaO.

关键词: Carbon monoxide, Zeolite, Catalyst, Dimethyl carbonate, Oxidative carbonylation, Dehydrating agent

Abstract: The influence of the dehydration by metal oxides on the synthesis of dimethyl carbonate (DMC) via oxidative carbonylation of methanol was studied. A Cu/Y-zeolite catalyst was prepared by the ion exchange method from CuCl₂·2H₂O and the commercial NH₄-form of the Y type zeolite. The catalyst was characterized by X-ray fluorescence (XRF), N2 adsorption (BET method), X-ray diffraction (XRD), and temperature-programmed desorption of ammonia (NH₃-TPD) to evaluate its Cu and Cl content, surface area, structure, and acidity. Reaction tests were carried out using an autoclave (batch reactor) for 18 h at 403 K and 5.5 MPa (2CH₃OH + 1/2O₂ + CO ? (CH₃O)₂CO + H₂O). The influence of various dehydrating agents (ZnO, MgO, and CaO) was examined with the aim of increasing the methanol conversion (X_MeOH, MeOH conversion). The MeOH conversion increased upon addition of metal oxides in the order CaO >> MgO > ZnO, with the DMC selectivity (S_DMC) following the order MgO > CaO > ZnO. The catalysts and dehydrating agents were characterized before and after the oxidative carbonylation of methanol by thermogravimetric and differential thermogravimetric (TG/DTG), and XRD to confirm that the dehydration reaction occurred via the metal oxide (MO + H₂O → M(OH)₂). The MeOH conversion increased from 8.7% to 14.6% and DMC selectivity increased from 39.0% to 53.1%, when using the dehydrating agent CaO.

Key words: Carbon monoxide, Zeolite, Catalyst, Dimethyl carbonate, Oxidative carbonylation, Dehydrating agent

Dong-Ho Lee, Jiin You, Je-Min Woo, Jung Yoon Seo, Young Cheol Park, Jong-Seop Lee, Hyunuk Kim, Jong-Ho Moon, Seung Bin Park. Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst[J]. Chinese Journal of Chemical Engineering, 2018, 26(5): 1059-1063.

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Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst

Influence of dehydrating agents on the oxidative carbonylation of methanol for dimethyl carbonate synthesis over a Cu/Y-zeolite catalyst

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