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One-step synthesis of methylal via methanol oxidation by Mo:Fe(x)/HZSM-5 bifunctional catalyst

机译:Mo:Fe(x)/ HZSM-5双功能催化剂通过甲醇氧化一步合成甲缩醛

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摘要

The traditional one-step process for preparing methylal bifunctional catalyst has multiple limitations, including high cost, high acidity and low yield. In order to overcome these limitations, the author designed and studied a series of Mo:Fe(x)/HZSM-5 function catalyst with different ferromolybdenum ratios. The one-step process for preparing methyl acetal is realized in a fluidized bed reactor. The effect of different ferromolybdenum ratios on its catalytic performance was investigated and the optimum ferromolybdenum ratio catalyst was found. The results show that this new process and catalyst can overcome the disadvantages of traditional bifunctional catalysts and achieve a relatively high DMM yield. For instance, the methanol conversion ratio and DMM selectivity of the Mo:Fe(2)/HZSM-5 bifunctional catalyst reached 87.44% and 93%, respectively. Moreover, the recorded DMM yield was 81.32%, which was much higher than that of other research results. At the same time, the XPS catalyst activity and activation energy results show that increased molybdenum loading catalytic effect. However, when Mo/Fe > 2, the mutual promotion effect would be larger and part of the formaldehyde obtained by oxidative dehydrogenation of methanol would be further oxidized to obtain the by-product formic acid, further producing more methyl formate. In addition, the self-made Mo:Fe(2)/HZSM-5 dual-functional catalyst exhibits high stability and carbon deposition resistance under severe operating conditions, compared to other bifunctional catalysts of this process.
机译:传统的一步制备甲基双功能催化剂的方法具有许多局限性,包括高成本,高酸度和低产率。为了克服这些限制,作者设计并研究了一系列具有不同钼铁比的Mo:Fe(x)/ HZSM-5功能催化剂。在流化床反应器中实现了一步制备甲基乙缩醛的方法。研究了不同比例的钼铁对其催化性能的影响,找到了最佳的钼钼比催化剂。结果表明,这种新方法和催化剂可以克服传统双功能催化剂的缺点,并获得较高的DMM收率。例如,Mo:Fe(2)/ HZSM-5双功能催化剂的甲醇转化率和DMM选择性分别达到87.44%和93%。此外,记录的DMM产率为81.32%,远高于其他研究结果。同时,XPS催化剂的活性和活化能结果表明,钼负载量增加了催化作用。然而,当Mo / Fe> 2时,相互促进作用将更大,并且通过甲醇的氧化脱氢获得的甲醛的一部分将被进一步氧化以获得副产物甲酸,从而进一步产生更多的甲酸甲酯。此外,与该方法的其他双功能催化剂相比,自制的Mo:Fe(2)/ HZSM-5双功能催化剂在苛刻的操作条件下显示出高稳定性和抗碳沉积性。

著录项

  • 来源
    《Fuel》 |2020年第1期|116416.1-116416.9|共9页
  • 作者单位

    China Univ Petr East China State Key Lab Heavy Oil Proc Qingdao 266580 Shandong Peoples R China;

    Xian Shiyou Univ Res Ctr Petr Proc & Petrochem Xian 710065 Shaanxi Peoples R China;

    Shandong Univ Sci & Technol Key Lab Low Carbon Energy & Chem Engn Qingdao 266590 Shandong Peoples R China;

    China Univ Petr East China State Key Lab Heavy Oil Proc Qingdao 266580 Shandong Peoples R China|Shandong Univ Sci & Technol Key Lab Low Carbon Energy & Chem Engn Qingdao 266590 Shandong Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Bifunctional catalyst; Mo:Fe(x)/HZSM-5; Methanol; Dimethoxymethane;

    机译:双功能催化剂;Mo:Fe(x)/ HZSM-5;甲醇;二甲氧基甲烷;

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