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Selective Carbonylation of Dimethyl Ether to Methyl Acetate Catalyzed by Acidic Zeolites

Selective Carbonylation of Dimethyl Ether to Methyl Acetate Catalyzed by Acidic Zeolites. Huimin Zhan 2013.7.19. Background. CH 3 OCH 3 +CO CH 3 COOCH 3. Catalyst ：. 400-500K ， 1.5MPa. CH 3 OCH 3 +CO CH 3 COOCH 3. H-MOR.

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Selective Carbonylation of Dimethyl Ether to Methyl Acetate Catalyzed by Acidic Zeolites

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  1. Selective Carbonylation of Dimethyl Ether to Methyl Acetate Catalyzed by Acidic Zeolites Huimin Zhan 2013.7.19

  2. Background CH3OCH3+CO CH3COOCH3 Catalyst：

  3. 400-500K，1.5MPa CH3OCH3+CO CH3COOCH3 H-MOR -Mild reaction condition -Non-noble metal catalyst，selectivity＞99% -Highly atom-economic -Less by-product

  4. Mechanism Study DME pulsing studies： DME and water were detected in the effluent during subsequent He treatment

  5. DME–CO mixtures DME–CO mixtures Pure CO

  6. Technology Condition CO/H2/DME=72/18/10 DME:CO=1:46.5 CO/H2/DME=76/19/5

  7. Catalyst Undetectable on H-USY (Si/Al=3:1), H-BEA (Si/Al=12.5:1), and amorphous SiO2–Al2O3 (Si/Al=3:1)

  8. outside the 8MR more accessible to 12MRchannel inside the 8MR

  9. Distribution of H+ Sites in MOR Propane : absorbed on sites located only within 8-MR channels n-Hexane : absorbed on sites located only within 12-MR channels ~3610cm : H+ in 12-MR channels ~3590cm : H+ in 8-MR channels

  10. Distribution of H+ Sites in Cation-Exchanged MOR Samples Na + exchange occurred selectively by replacement of H+ within 8-MR side pockets Co2+ replaced H+ with similar probability in 8-MR and 12-MR channels

  11. The Synthesis of Catalyst Pyt：吡咯烷；TMA：四甲基铵；HMI：环己亚胺

  12. Pre-adsorption of Pyridine HOMR-6、Py-HMOR-6：Si/Al=6 ;HMOR-10、Py-HMOR-10：Si/Al=10

  13. The Addition of Methyl Acetate or Acetic Acid in Reactant

  14. Selective Dealumination of Mordenite The method of dealumination : pyridine aqueous NaOH solution calcine Py-Na-MOR H-MOR Py-HMOR aqueous NaOH solution NH4NO3 ion-exchange 1023K H-Na-MOR a gas stream of 30% H2O calcine HMOR-1023 NH4-MOR

  15. (NH4)2SiF6 The selective removal of aluminium from the 12-membered ring channels and also from the surface of the zeolite. A：MOR B：MOR (NH4)2SiF6

  16. Selective Extraction of Silicon NaOH、NH4OH： The selective extraction of silicon from a zeolite framework

  17. Cu/H-MOR Cu loading amount : 4.7wt% The location exchange of proton with Cu2+ after ion-exchange treatment

  18. Cu loading amount：Catalyst B ——15mol%；Catalyst E——59mol% Reaction condition：300℃，70bar，GHSV=4000h-1，CO/H2/DME=72/18/10

  19. The Impact of Particle Size and Crystal Size The carbonylation of dimethyl ether Particle size ：2-3.5μm

  20. The carbonylation of methanol Crystal size：Catalyst I——0.1-0.5μm ；Catalyst J——3-7 μm Crystal size ：0.1-1.5 μm

  21. HZSM-35

  22. Work Plan 研究内容： 硅铝比，比表面积和孔分布，酸性及酸量，晶粒大小和颗粒尺寸等对羰基化的影响 工作计划： 1、尝试合成丝光沸石，实现不同硅铝比、酸量、晶粒尺寸等丝光沸石的可控制备 2、寻找合适的丝光沸石处理方法，对工业丝光沸石进行改性，制备性能更优良的催化剂 3、调试设备，考察反应工艺条件

  23. Thanks for Your Attention! Qs & As

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