Volume 40 Issue 10
Oct.  2012
Turn off MathJax
Article Contents
WANG Zeng-zhu, HUANG Shou-ying, SHEN Yong-li, WANG Sheng-ping, MA Xin-bin. In situ DRIFTS study on the oxidative carbonylation of methanol to dimethyl carbonate over Cuβ catalyst[J]. Journal of Fuel Chemistry and Technology, 2012, 40(10): 1212-1221.
Citation: WANG Zeng-zhu, HUANG Shou-ying, SHEN Yong-li, WANG Sheng-ping, MA Xin-bin. In situ DRIFTS study on the oxidative carbonylation of methanol to dimethyl carbonate over Cuβ catalyst[J]. Journal of Fuel Chemistry and Technology, 2012, 40(10): 1212-1221.

In situ DRIFTS study on the oxidative carbonylation of methanol to dimethyl carbonate over Cuβ catalyst

  • Received Date: 2012-03-27
  • Rev Recd Date: 2012-05-25
  • Publish Date: 2012-10-31
  • The mechanism of oxidative carbonylation of methanol to dimethyl carbonate (DMC) over Cuβ catalyst was investigated by using in situ DRIFTS; the adsorption of single methanol, carbon monoxide and DMC as well as their mixtures on the Cuβ catalyst were considered. The results indicated that methoxide species are formed when methanol is adsorbed on the catalyst due to presence of CuO<em>x. Only one type of active sites that are located in the six-membered ring of β zeolite is found, over which adsorbed methanol can be oxidized to methoxide and water. DMC is adsorbed on the catalyst through the contact of the oxygen atom in carbonyl group with the active sites. There were two pathways for the oxidative carbonylation: by the mono-methoxide pathway, carbon monoxide can react with mono-methoxide species to form monomethyl carbonate (MMC) and MMC then reacts with methoxide to form DMC, or by the di-methoxide pathway, DMC is formed through inserting of carbon monoxide in the di-methoxide species; latter one is more favorable over the Cuβ catalyst.
  • loading
  • PACHECO M A, MARSHALL C L. Review of dimethyl carbonate (DMC) manufacture and its characteristics as a fuel additive[J]. Energy Fuels, 1997, 11(1): 2-29.
    KELLER N, REBMANN G, KELLER V. Catalysts, mechanisms and industrial processes for the dimethylcarbonate synthesis[J]. J Mol Catal A,2010, 317(1/2): 1-18.
    DELLEDONNE D, RIVETTI F, ROMANO U. Developments in the production and application of dimethylcarbonate[J]. Appl Catal A, 2001, 221(1/2): 241-251.
    马新宾, 黄守莹, 王胜平, 张萍波. 氧化羰基化法合成有机碳酸酯的研究进展[J]. 石油化工,2010, 9(7): 697-705. (MA Xin-bin, HUANG Shou-ying, WANG Sheng-ping, ZHANG Ping-bo. Advance in synthesis of organic carbonate by oxidative carbonylation[J]. Petrochemical Technology, 2010, 39(7): 697-705.)
    李其明,李芳. 碳酸二甲酯合成的研究进展[J]. 化学试剂,2011, 33(4): 321-324. (LI Qi-ming, LI Fang. Research progress on synthesis of dimethyl carbonate[J]. Chemical Reagent, 2011, 33(4): 321-324.)
    ANDERSON S. Kinetic studies of carbonylation of methanol to dimethyl carbonate over Cu+X zeolite catalyst[J]. J Catal, 2003, 217(2): 396-405.
    KING S T. Reaction mechanism of oxidative carbonylation of methanol to dimethyl carbonate in Cu-Y zeolite[J]. J Catal, 1996, 161(2): 530-538.
    ZHANG Y, BELL A T. The mechanism of dimethyl carbonate synthesis on Cu-exchanged zeolite Y[J]. J Catal, 2008, 255(2): 153-161.
    ENGELDINGER J, DOMKE C, RICHTER M, BENTRUP U. Elucidating the role of Cu species in the oxidative carbonylation of methanol to dimethyl carbonate on CuY: An in situ spectroscopic and catalytic study[J]. Appl Catal A, 2010, 382(2): 303-311.
    ENGELDINGER J, RICHTER M, BENTRUP U. Mechanistic investigations on dimethyl carbonate formation by oxidative carbonylation of methanol over a CuY zeolite: An operando SSITKA/DRIFTS/MS study[J]. Phys Chem Chem Phys, 2012, 14(7): 2183
    ZHANG Y, BRIGGS D N, de SMIT E, BELL A T. Effects of zeolite structure and composition on the synthesis of dimethyl carbonate by oxidative carbonylation of methanol on Cu-exchanged Y, ZSM-5, and Mordenite[J]. J Catal, 2007, 251(2): 443-452.
    ZHANG P, HUANG S, YANG Y, MENG Q, WANG S, MA X. Effect of SSIE structure of Cu-exchanged β and Y on the selectivity for synthesis of diethyl carbonate by oxidative carbonylation of ethanol: A comparative investigation[J]. Catal Today, 2010, 149(1/2): 202-206.
    ZHANG P, HUANG S, WANG S, MA X. Effect of extra-framework silicon on the catalytic activity of Cuβ zeolite catalyst for synthesis of diethyl carbonate by oxidative carbonylation of ethanol[J]. Chem Eng J, 2011, 172(1): 526-530.
    GRUVER V, PANOV A, FRIPIAT J J. Infrared study of CO chemisorbed on Brönsted and Lewis sites in dealuminated acid Y and ZSM-5 zeolites[J]. Langmuir, 1996, 2(10): 2505-2513.
    MINTOVA S, VALTCHEV V, ONFROY T, MARICHAL C, KNÖZINGER H, BEIN T. Variation of the Si/Al ratio in nanosized zeolite Beta crystals[J]. Microporous Mesoporous Mater, 2006, 90(1/3): 237-245.
    DAVYDOV A A, BUDNEVA A A. IR spectra of CO and NO adsorbed on CuO[J]. React Kinet Catal Lett, 1984, 25(1/2): 121-124.
    BUSCA G. FT-IR study of the surface of copper oxide[J]. J Mol Catal, 1987, 43(2): 225-236.
    NEWSAM J M, TREACY M M J, KOETSIER W T, de GRUYTER C B. Structural characterization of zeolite beta[J]. Proceedings of The Royal Society of London, Series A: Mathematical and Physical Sciences, 1988, 420(1859): 375-405.
    LI P, XIANG Y, GRASSIAN V H, LARSEN S C. CO adsorption as a probe of acid sites and the electric field in alkaline earth exchanged zeolite beta using FT-IR and ab Initio quantum calculations[J]. J Phys Chem B, 1999, 103(24): 5058-5062.
    BEUTEL T. Spectroscopic and kinetic study of the alkylation of phenol with dimethyl carbonate over NaX zeolite[J]. J Chem Soc Faraday Trans, 1998, 94(7): 985-993.
    KUKULSKA-ZAJAC E, DATKA J. Transformations of formaldehyde molecules in Cu-ZSM-5 zeolites[J]. J Phys Chem C, 2007, 111(8): 3471-3475.
    余运波, 贺泓. Ag/Al2O3选择性催化丙烯还原氮氧化物表面反应机理的原位红外光谱研究[J]. 催化学报, 2003, 24(5): 385-390. (YU Yun-bo, HE Hong. Mechanistic study of lean NO reduction with propene over Ag/Al2O3 by in situ DRIFTS[J]. Chinese Journal of Catalysis, 2003, 24(5): 385-390.)
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索

    Article Metrics

    Article views (2175) PDF downloads(872) Cited by()
    Proportional views
    Related

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return