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Switching Between Oxidation Types Using Molybdenum Phosphate Catalysts for Paraffin Activation Using Doped Fe as Surface Acidity Modifier and MoOx as an Oxygen Insertion Tool
Catalysis Letters ( IF 2.3 ) Pub Date : 2019-09-17 , DOI: 10.1007/s10562-019-02943-z
Zibuyile Mncwabe , Majid D. Farahani , Holger B. Friedrich

A comparative study of the activation of n-hexane over 12-molybdophopshoric acid (H3PMo12O40 or HPA), Fe3+ doped HPA (Fe0.69H0.93PMo12O40) and an iron phosphate catalyst (P/Fe = 1.22) was carried out. The Fe doped HPA catalyst is thermally more stable and less acidic than the unmodified HPA catalyst. The HPA and the Fe doped HPA catalysts both catalytically produced 2,5-dimethyltetrahydrofuran and 2,5-hexadione (oxygenates), with the Fe doped HPA catalyst selectively producing more oxygenates than the HPA catalyst. The iron phosphate catalyst produced cis-2-hexene and 1-hexene but no oxygenates, which implies that the iron phosphate catalyst promotes dehydrogenation, but not oxygen insertion. At 360 °C, the HPA catalyst initiated benzene formation reactions. At isoconversion of ca. 8% under isothermal conditions, the iron phosphate catalyst gave the highest selectivity (72%) towards benzene, which may have formed through both catalytic and non-catalytic reactions. In contrast, the Fe doped HPA catalyst showed a lower benzene selectivity than the HPA catalyst with a corresponding increase in cyclic oxygenates.

中文翻译:

使用磷酸钼催化剂进行石蜡活化,使用掺杂的 Fe 作为表面酸度改性剂和 MoOx 作为氧插入工具在氧化类型之间切换

对正己烷在 12-钼磷酸(H3PMo12O40 或 HPA)、Fe3+ 掺杂的 HPA(Fe0.69H0.93PMo12O40)和磷酸铁催化剂(P/Fe = 1.22)上的活化进行了比较研究。与未改性的 HPA 催化剂相比,Fe 掺杂的 HPA 催化剂在热上更稳定且酸性更小。HPA 和 Fe 掺杂的 HPA 催化剂均催化产生 2,5-二甲基四氢呋喃和 2,5-己二酮(含氧化合物),Fe 掺杂的 HPA 催化剂选择性地产生比 HPA 催化剂更多的含氧化合物。磷酸铁催化剂产生顺式 2-己烯和 1-己烯,但没有含氧化合物,这意味着磷酸铁催化剂促进脱氢,但不促进氧插入。在 360 °C 时,HPA 催化剂引发苯形成反应。在约的等转化。等温条件下 8%,磷酸铁催化剂对苯的选择性最高 (72%),苯可能是通过催化和非催化反应形成的。相比之下,Fe 掺杂的 HPA 催化剂显示出比 HPA 催化剂更低的苯选择性,相应地增加了环氧化物。
更新日期:2019-09-17
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