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Isomerisation of n-hexane over bifunctional Pt-heteropoly acid catalyst: Enhancing effect of gold
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-11-21 , DOI: 10.1016/j.jcat.2017.11.001
Abdulrahman Alazman , Domagoj Belic , Elena F. Kozhevnikova , Ivan V. Kozhevnikov

Isomerisation of n-hexane was studied in the presence of acid and bifunctional metal-acid catalysts based on Keggin-type heteropoly acids (HPA), in particular focusing on Cs2.5H0.5PW12O40 (CsPW) and Pt/CsPW as the catalysts, using a fixed-bed microreactor under differential conditions (n-hexane conversion ≤ 10%) at 180–220 °C, ambient pressure and a ratio of n-hexane and H2 partial pressures of 0.06–0.24. The turnover rate of HPA-catalysed isomerisation was found to correlate with the acid strength of HPA (initial enthalpy of ammonia adsorption). Bifunctional Pt-HPA catalysts were more efficient than monofunctional HPA catalysts. In the isomerisation over Pt/CsPW bifunctional catalyst, n-hexane dehydrogenation step was found to equilibrate at a molar ratio of Pt and H+ surface sites Pts/H+ ≥ 0.8, corresponding to a Pt loading ≥6%. Bimetallic PtAu/CsPW catalyst showed higher activity in n-hexane isomerisation than Pt/CsPW, although the Au alone without Pt was inert. In the presence of Au, the turnover rate at Pt sites increased more than twofold. The effect of Au is attributed to PtAu alloying. Scanning transmission electron microscopy–energy dispersive X-ray spectroscopy (STEM-EDX) and X-ray diffraction (XRD) analyses of PtAu/CsPW indicated the presence of bimetallic PtAu nanoparticles with a wide range of Pt/Au atomic ratios.



中文翻译:

的异构化Ñ己烷双官能以上的Pt-杂多酸催化剂:提高的效果金

的异构化ñ -己烷在基于Keggin型杂多酸(HPA)酸和双官能金属酸催化剂的存在下的研究,特别着眼于铯2.5 ħ 0.5 PW 12 ø 40(CsPW)和Pt / CsPW作为催化剂,使用差的条件(下一个固定床微反应器ñ正己烷转化率≤10%)在180-220℃,环境压力和的比率ñ -己烷和H 2分压为0.06-0.24。发现HPA催化异构化的周转率与HPA的酸强度(氨吸附的初始焓)相关。双官能Pt-HPA催化剂比单官能HPA催化剂更有效。在异构化在Pt / CsPW双功能催化剂,Ñ己烷脱氢步骤被发现在Pt和H的摩尔比以平衡+表面位点的Pt小号/ H +  ≥0.8,对应于Pt负载≥6%。双金属PtAu / CsPW催化剂在n中表现出更高的活性-己烷异构化比Pt / CsPW异构化,尽管没有Pt的单独的Au是惰性的。在金的存在下,铂位点的周转率增加了两倍以上。Au的作用归因于PtAu合金化。扫描透射电子显微镜–能量色散X射线能谱(STEM-EDX)和X射线衍射(XRD)分析PtAu / CsPW表明存在双金属PtAu纳米粒子,具有宽范围的Pt / Au原子比。

更新日期:2017-11-21
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