Vapor Phase Carbonylation of Methanol to Acetic Acid with Pressurized Fluidyzed Bed Reactor

加压流化床反应器气相羰基化甲醇制乙酸

基本信息

  • 批准号:
    59850139
  • 负责人:
  • 金额:
    $ 13.12万
  • 依托单位:
  • 依托单位国家:
    日本
  • 项目类别:
    Grant-in-Aid for Developmental Scientific Research
  • 财政年份:
    1984
  • 资助国家:
    日本
  • 起止时间:
    1984 至 1986
  • 项目状态:
    已结题

项目摘要

It was found that a nickel on active carbon (Ni/A.C.) catalyst exhibited a high activity and selectivity for the vapor phase carbonylation of methanol to acetic acid under moderately pressurized (5-30 atm) and heated (200-300 ゜C) conditions. The 2.5% Ni/A.C. catalyst gave ; 100% methanol conversion and 97% acetic acid yield, in the presence of methyl iodide promoter and excess carbon monoxide. The reaction path was clarified as follows: The yield of each product as a function of time factor was well simulated by calculating numerically the rate of each unit reaction. The Ni/A.C. catalyst was stable during the reaction, which exhibited a half life time of 50 days. The decrease in the catalytic activity was not attributed to the vaporization of nickel from the catalyst but to the deposition of tarry material on the catalyst, which caused the plugging of micro-pores in the catalyst.A fluidized bed reactor, which was able to be operated under pressurized conditions with a gas-recycle, was built and subjected to the methanol carbonylation. A remarkable flat temperature profile was attained in the catalyst bed during the reaction, which gave a result of more than 1 Kg-acetic acid/Kg-cat.h with a selectivity of 99% carbonylated products. The level is even superior to that of a fixed bed reaction and is sufficient for industrialization.It was also found that hydrogen in the feed gas, which commonly exist in CO, remarkably promotes the reaction with little change in the product selectivity. The hydrogen did not promote any particular reaction but promoted all reactions in the reaction network. However, little hydrogen in the gas phase was not incorporated in the product, suggesting that the promotional effect being not in the direct way but in the indirect way.The feasibility study of the present process suggests that it is competitive to a presently operating process which uses rhodium catalyst.
研究发现,活性炭镍(Ni/A.C.)催化剂在中等压力(5-30 atm)和加热(200-300 ゜C)条件下对甲醇气相羰基化制乙酸表现出高活性和选择性。 2.5% Ni/A.C.催化剂给出;在碘甲烷促进剂和过量一氧化碳存在下,甲醇转化率为 100%,乙酸收率为 97%。反应路径阐明如下:通过数值计算每个单元反应的速率,很好地模拟了每个产物的收率作为时间因素的函数。 Ni/A.C.催化剂在反应过程中稳定,半衰期为50天。催化活性的下降并不是由于催化剂中镍的蒸发,而是由于焦油状物质在催化剂上的沉积,导致催化剂微孔的堵塞。搭建了一个能够在加压条件下操作并具有气体循环的流化床反应器,并进行了甲醇羰基化反应。反应过程中催化剂床中的温度曲线非常平坦,产生了超过 1 Kg-乙酸/Kg-cat.h 的结果,且羰基化产物的选择性为 99%。该水平甚至优于固定床反应,足以工业化。我们还发现,原料气中的氢气(通常存在于CO中)显着促进了反应,而产物选择性几乎没有变化。氢气不促进任何特定反应,但促进反应网络中的所有反应。然而,气相中的少量氢气没有并入产物中,这表明促进作用不是直接方式而是间接方式。本工艺的可行性研究表明,它与目前使用铑催化剂的操作工艺相比具有竞争力。

项目成果

期刊论文数量(15)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
K.Fujimoto, K.Omata, T.Shikada, H.Tominaga: American Chemical Society. Industrial Chemicals via C1 Processes, 208 (1987)
K.Fujimoto、K.Omata、T.Shikada、H.Tominaga:美国化学会。
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    0
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Ind.Eng.Chem.Prod.Res.Dev.22-3. (1983)
工业工程化学产品研究开发 22-3。
  • DOI:
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    0
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K.Fujimoto;K.Omata;T.Shikada;H.Tominaga: "Industrial Chemicals via C1 Processes" American Chemical Society, 261 (1987)
K.Fujimoto;K.Omata;T.Shikada;H.Tominaga:“通过 C1 工艺生产工业化学品”美国化学会,261 (1987)
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    0
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  • 通讯作者:
T. Shikada, H. Yagita, K. Omata, K. Fujimoto, and H. Tominaga: "Vapor Phase Carbonylation of Organic Compound over Supported Transition Metal Catalysts. 4.Synthesis of Acetic Anhydride from Methyl Acetate with Nickel Active Carbon Catalyst" Ind. Eng. Chem
T. Shikada、H. Yagita、K. Omata、K. Fujimoto 和 H. Tominaga:“有机化合物在负载型过渡金属催化剂上的气相羰基化。4.用镍活性炭催化剂从乙酸甲酯合成乙酸酐”Ind
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    0
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  • 通讯作者:
K.Omata;K.Fujimoto;T.Shikada;H.Tominaga: Ind.Eng.Chem.Prod.Res.Dev.24. 234-239 (1985)
K.Omata;K.Fujimoto;T.Shikada;H.Tominaga:Ind.Eng.Chem.Prod.Res.Dev.24。
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TOMINAGA Hiro-o其他文献

TOMINAGA Hiro-o的其他文献

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{{ truncateString('TOMINAGA Hiro-o', 18)}}的其他基金

Japan - Germany Joint Research on Cl Chemistry
日德氯化学联合研究
  • 批准号:
    01044042
  • 财政年份:
    1989
  • 资助金额:
    $ 13.12万
  • 项目类别:
    Grant-in-Aid for international Scientific Research
Application of Laser to Selective Partial Oxidation of Hydrocarbons by Dioxygen
激光在分子氧选择性部分氧化碳氢化合物中的应用
  • 批准号:
    63430017
  • 财政年份:
    1988
  • 资助金额:
    $ 13.12万
  • 项目类别:
    Grant-in-Aid for General Scientific Research (A)

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