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Organophosphorous surfactant-assistant synthesis of SAPO-34 molecular sieve with special morphology and improved MTO performance

机译:有机磷表面活性剂 - 辅助合成SAPO-34分子筛具有特殊形态,改善MTO性能

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With the aid of self-designed organophosphorous surfactant [2-(diethoxylphosphono)propyl]hexadecyldimethylammonium bromide (DPHAB), SAPO-34s with various special morphologies have been hydrothermally synthesized by using tetraethylammonium hydroxide (TEAOH), diethylamine (DEA) and triethylamine (TEA) as templates, respectively. The synthesized SAPO-34s were well characterized by XRD, XRF, SEM, N _(2) adsorption–desorption, solid state NMR and NH _(3) -TPD measurements. The status of DPHAB was also investigated by using FT-IR, ~(13) C NMR, TG–DTA and ~(31) P NMR measurements as well as density functional theory calculations. It is found that the addition of DPHAB changes the crystal morphology dramatically and the aggregation degree of the crystals increases with the rising DPHAB/H _(3) PO _(4) ratio. Moreover, microporous templates play an important role in the synthesis of mesoporous SAPO-34. TEAOH, which has the strongest interaction energy with the CHA framework among the investigated templates, shows the best cooperating ability with an organophosphorous surfactant to direct the formation of nanosized and mesoporous SAPO-34. The prepared SAPO-34s showed improved catalytic properties in the methanol-to-olefins (MTO) reaction.
机译:借助自行设计的有机磷表面活性剂[2-(二乙氧基膦酰基膦)丙基溴铵(DPHAB),通过使用四乙基氢氧化铵(Teah),二乙胺(DEA)和三乙胺(茶叶分别为模板。通过XRD,XRF,SEM,N _(2)吸附 - 解吸,固态NMR和NH _(3)-TPD测量,合成的SAPO-34S表征很好。通过使用FT-IR,〜(13)C NMR,TG-DTA和〜(31)P NMR测量以及密度泛函理论计算,还研究了DPHAB的状态。发现DPHAB的添加显着改变晶体形态,并且晶体的聚集度随着上升的DPHAB / H _(3)PO _(4)比而增加。此外,微孔模板在介孔SAPO-34的合成中发挥着重要作用。在调查模板中具有最强的相互作用能量的Teah,表明了具有有机磷表面活性剂的最佳合作能力,以指导纳米化和中孔SAPO-34的形成。制备的SAPO-34s显示出甲醇 - 烯烃(MTO)反应中的改善的催化性质。

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