Effects of Anion Substitution in (Mo,V)5O14 on Catalytic Performance in Selective Propene Oxidation to Acrolein

Effects of Anion Substitution in (Mo,V)5O14 on Catalytic Performance in Selective Propene Oxidation to Acrolein
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(Mo,V)5O14 阴离子取代对丙烯选择性氧化制丙烯醛催化性能的影响

DOI:
10.1002/cctc.201501076
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发表时间:
2016
期刊:
影响因子:
4.5
通讯作者:
T. Ressler
T. Ressler
中科院分区:
化学3区
文献类型:
--
作者:
S. Kuhn;D. Weber;M. Lerch;T. Ressler

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钼基混合氧化物代表了众所周知的轻质烯烃选择性氧化模型催化剂。在此,首次通过用氮离子取代氧离子来修饰(Mo,V)5O14的阴离子晶格。 XRD 分析、X 射线吸收光谱和 FTIR 光谱研究表明,氮在 Mo5O14 结构中的掺入并未改变金属中心的平均价态。此外,阻抗谱证实了氧空位的形成。除去氮后电导率仍然存在显着变化。进行程序升温还原测量以研究氧迁移率。氮氧化物还原性的增强与电导率的增加相关。通过在线质谱和气相色谱在不同温度下测定选择性丙烯氧化的催化性能。随着电导率的增加,对丙烯醛的选择性增加,而总氧化产物COx的形成减少。
Molybdenum‐based mixed oxides represent well‐known model catalysts for the selective oxidation of light alkenes. Here, the anion lattice of (Mo,V)5O14was for the first time modified by substituting oxygen ions with nitrogen ions. Investigations by XRD analysis, X‐ray absorption spectroscopy, and FTIR spectroscopy revealed that the incorporation of nitrogen in the structure of Mo5O14proceeded without changing the average valence of metal centers. Additionally, impedance spectroscopy confirmed the formation of oxygen vacancies. Significant changes in conductivities remained after the removal of nitrogen. Temperature‐programmed reduction measurements were performed to investigate oxygen mobility. The enhanced reducibility of oxide nitrides correlated with the increased conductivity. Catalytic performance in selective propene oxidation was determined by online mass spectrometry und gas chromatography at different temperatures. Selectivity towards acrolein increased with increasing conductivity whereas the formation of total oxidation products COxdecreased.
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