Effects of the support on bifunctional one-step synthesis of methylal via methanol oxidation catalysed by Fe–Mo-based bifunctional catalysts,Sustainable Energy & Fuels

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Effects of the support on bifunctional one-step synthesis of methylal via methanol oxidation catalysed by Fe–Mo-based bifunctional catalysts
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2020-11-04 , DOI: 10.1039/d0se01194k
Meng Yuan _{1,

2,

3,

4,

5} , Ruiyuan Tang _{4,

6,

7,

8} , Xiangyu Sun _{2,

9,

10,

11} , Zhimei Zhang _{1,

2,

3,

4,

5} , Yuanyu Tian _{1,

2,

3,

4,

5} , Yingyun Qiao _{1,

2,

3,

4,

5}

Affiliation

In the one-step preparation of methylal from methanol, achieving high methanol conversion and high methylal yield is a huge challenge. To address this problem, in this study a new Fe–Mo-based catalyst was designed, and the effect of the type and amount of the support on catalytic activity was explored. The results showed that Mo:Fe(2)/HZSM-5(80 + 80), in which HZSM-5(80 + 80) was the catalytic support, had excellent catalytic performance, with the yield of methylal reaching 81.33%, much higher than other reported results of this process. Through XPS, NH₃-TPD and PY-FTIR analyses it was found that the formation of Mo⁵⁺ promoted coordination of the two terminal oxygens with the Mo double bond in the Fe₂(MoO₄)₃ octahedron, and the higher the B/L acid site ratio, the better the catalytic activity and the higher the selectivity of the target product. The apparent activation energy also further proved that Mo:Fe(2)/HZSM-5(80 + 80) was highly suitable for the one-step production of methylal from methanol.

中文翻译：

载体对Fe-Mo基双功能催化剂催化甲醇氧化双功能一步合成甲缩醛的影响

在由甲醇一步制备甲醇中，实现高甲醇转化率和高甲醇收率是巨大的挑战。为了解决这个问题，在本研究中，设计了一种新的基于Fe-Mo的催化剂，并研究了载体类型和载体量对催化活性的影响。结果表明，以HZSM-5（80 + 80）为催化载体的Mo：Fe（2）/ HZSM-5（80 + 80）具有优异的催化性能，甲缩醛的收率达到81.33％，非常高。高于此过程的其他报告结果。通过XPS，NH ₃ -TPD和PY-FTIR分析，发现Mo ⁵⁺的形成促进了Fe ₂（MoO ₄）_3中两个末端氧与Mo双键的配位。八面体，B / L酸位点比率越高，催化活性越好，目标产物的选择性也越高。表观活化能还进一步证明Mo：Fe（2）/ HZSM-5（80 + 80）非常适合从甲醇一步一步生产甲缩醛。

更新日期：2020-11-21

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