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n-Hexane hydroisomerization over Zr-modified bicontinuous lamellar silica mordenite supported Pt as highly selective catalyst: Molecular hydrogen generated protonic acid sites and optimization
International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2020-11-24 , DOI: 10.1016/j.ijhydene.2020.11.006
M. Ibrahim , A.A. Jalil , W.F.W. Zakaria , N.A.A. Fatah , M.Y.S. Hamid , S.M. Izan , H.D. Setiabudi

Zr-modified bicontinuous lamellar silica mordenite supported Pt catalysts were synthesized using the zirconyl chloride oxahydrate as the precursor for Zr species by the incipient wetness impregnation method. The influence of zirconium loading on the properties of Zr-modified HM@KCC-1 catalysts for n-hexane isomerization were studied. The results of XRD and lattice structure from IR study indicated that increasing zirconium loading did not change the properties of catalysts. The IR study with pre-adsorbed 2,6-dimethylpyridine as a probe molecule affirmed that increasing zirconium loading could increase the Lewis acid sites. The generation of protonic acid sites which were active in n-hexane hydroisomerization was mainly from molecular hydrogen through a hydrogen spill-over mechanism as established by in situ-IR study. The results for the catalytic testing indicated that PtZr/HM@KCC-1 catalyst was highly selective in n-hexane hydroisomerization due to abundant permanent Lewis acid sites for its promotive effect in the generation of protonic acid sites. However, the incorporation of excessive zirconium amount up to 10 wt percent loading led to a decline in the amount of protonic acid sites generated, thus reduced the hydroisomerization performance in the process. The optimum conditions for hydroisomerization of n-hexane over Pt5Zr/HM@KCC-1 were reaction temperature of 293 °C, treatment temperature of 474 °C and F/W of 502 mL/g.min with the predicted value for isomer yield of 83.9%.



中文翻译:

Ñ过的Zr改性的层状双连续丝光沸石的二氧化硅-己烷加氢异构化的Pt担载作为高选择性催化剂:生成分子氢质子酸位点和优化

以氧化锆氧杂水合物作为Zr物种的前体,通过初期湿润浸渍法合成了Zr改性的双连续层状二氧化硅丝光沸石负载的Pt催化剂。装载锆的锆上改性HM的@ KCC-1催化剂的性质的影响Ñ正己烷的异构化进行了研究。IR研究的XRD和晶格结构结果表明,增加锆负载量不会改变催化剂的性能。用预吸附的2,6-二甲基吡啶作为探针分子进行的红外研究证实,增加锆的负载量可以增加路易斯酸的位点。在n中有活性的质子酸位点的产生正己烷加氢异构化主要是由分子氢通过原位红外研究建立的氢溢出机理引起的。对于催化测试结果表明,PtZr / HM @ KCC-1催化剂是高度选择性Ñ正己烷加氢异构化由于在质子酸位点的产生的促进作用。丰富永久路易斯酸位点。但是,过量锆的掺入量高达10wt%,导致生成的质子酸位点的量减少,因此降低了该方法中的加氢异构化性能。n加氢异构化的最佳条件Pt5Zr / HM @ KCC-1上的正己烷反应温度为293°C,处理温度为474°C,F / W为502 mL / g.min,异构体收率的预测值为83.9%。

更新日期:2020-11-24
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