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首页> 外文期刊>CrystEngComm >Hollow nanocrystals of silicoaluminophosphate molecular sieves synthesized by an aminothermal co-templating strategy
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Hollow nanocrystals of silicoaluminophosphate molecular sieves synthesized by an aminothermal co-templating strategy

机译:氨基热共模板法合成硅铝磷酸盐分子筛的空心纳米晶体

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摘要

An aminothermal co-templating strategy has been developed to explore the synthesis of SAPO molecular sieves. Nanosized SAPO-56 (AFX) with a hollow morphology is, for the first time, obtained by utilizing triethylamine (TEA) and trimethylamine (TMA) as both the solvent and the template in the presence of HF. The prepared material is well characterized, and the coexistence of TEA and TMA in the crystals is proved by C-13 NMR. Molecular modelling indicates that the most stable status for the as-made SAPO-56 is 2TEA per aft cage and 1TMA per gme cage in the AFX structure, which is consistent with the TG results and verifies the co-templating behaviour of the two amines. In addition, the aminothermal crystallization process of SAPO-56 is examined, revealing an interesting in situ phase transformation from SAPO-34 (only containing TEA) to nano SAPO-56 followed by a further in situ post-synthetic leaching to achieve the hollow structure. Both F- anions and organic amines are proposed to be responsible for the dissolution of SAPO-34 and the etching of SAPO-56 nanocrystals. The Si-rich outer layer with abundant Si coordination environments (more Si-O-Al bonds and less Al-O-P bonds) helps the shell of SAPO-56 survive the leaching. This work offers an effective way to prepare SAPO-56 nanocrystals and demonstrates the huge potential of the aminothermal co-templating route for new material synthesis.
机译:已开发出氨基热共模板化策略以探索SAPO分子筛的合成。具有中空形态的纳米级SAPO-56(AFX)首次通过在氢氟酸存在下利用三乙胺(TEA)和三甲胺(TMA)作为溶剂和模板获得。所制备的材料具有良好的特性,并通过C-13 NMR证明了TEA和TMA在晶体中的共存。分子建模表明,制成的SAPO-56的最稳定状态是AFX结构中的每尾笼2TEA和每gme笼1TMA,这与TG结果一致,并验证了这两种胺的共模板化行为。此外,检查了SAPO-56的氨基热结晶过程,揭示了从SAPO-34(仅包含TEA)到纳米SAPO-56的有趣的原位相转变,然后进行了进一步的原位后合成浸出以实现中空结构。有人建议F-阴离子和有机胺都负责SAPO-34的溶解和SAPO-56纳米晶体的蚀刻。具有丰富的Si配位环境(更多的Si-O-Al键和更少的Al-O-P键)的富Si外层有助于SAPO-56的壳在浸出过程中存活下来。这项工作提供了一种制备SAPO-56纳米晶体的有效方法,并证明了氨基热共模板法在新材料合成中的巨大潜力。

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