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Sustainable synthesis of AEI/CHA intergrowth zeolites for methanol-to-olefins conversion
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2022-08-28 , DOI: 10.1016/j.micromeso.2022.112201
Zhihong Li , Yuanshuai Liu , Tao Dou , Xiaofeng Li , Chunyu Di , Sheng-Li Chen

The conventional hydrothermal synthesis of zeolites is inevitably accompanied by the production of mother liquors containing plentiful unreacted raw materials and organic templates. The direct emission or improper use of these mother liquors will cause not only the environmental contamination but also the waste of resources. Here we report a promising synthetic strategy for the effective recycle of mother liquors produced from the industrial production of SAPO-34 zeolites. Mother liquors with the addition of extra Si, P and Al were spray-dried and subsequently converted to the crystal seeds by vapor-phase-transport (VPT) method. Zeolite products with improved porosity and altered acidity were eventually acquired by VPT-Seeds-assisted hydrothermal crystallization, in which the topologic structures (e.g., CHA, AEI or AEI/CHA intergrowth) of zeolites depended significantly on the crystalline phase of VPT-Seeds. We demonstrated further via FT-IR and kinetics study that VPT-Seeds accelerated the crystallization of zeolites dramatically without the severe dissolution during the whole stage of synthesis. The as-synthesized AEI/CHA intergrowth zeolites showed the enhanced catalytic lifetime (increased at least by 27.6%) and higher selectivity in (C2H4+C3H6) (increased by 2.5%) during methanol-to-olefins (MTO) reactions than the pure CHA zeolites synthesized by the conventional hydrothermal method. Zeolites synthesized using the secondary recycled mother liquors in the same way also showed the comparable catalytic performances in MTO process, again verifying the feasibility of our methods to recycle mother liquors. The sustainable synthesis route developed in this work should be applicable to the industrial production of a wide variety of zeolites.



中文翻译:

用于甲醇制烯烃转化的 AEI/CHA 共生沸石的可持续合成

沸石的常规水热合成不可避免地伴随着母液的生产,该母液含有大量未反应的原料和有机模板。这些母液直接排放或使用不当,不仅会造成环境污染,还会造成资源浪费。在这里,我们报告了一种有前景的合成策略,用于有效回收 SAPO-34 沸石工业生产产生的母液。添加了额外的 Si、P 和 Al 的母液被喷雾干燥,随后通过气相传输 (VPT) 方法转化为晶种。最终通过 VPT-Seeds 辅助水热结晶获得了孔隙率提高和酸度改变的沸石产品,其中拓扑结构(例如 CHA、沸石的 AEI 或 AEI/CHA 共生)显着依赖于 VPT 种子的结晶相。我们通过 FT-IR 和动力学研究进一步证明,VPT-Seeds 显着加速了沸石的结晶,而在整个合成阶段没有严重的溶解。合成后的 AEI/CHA 共生沸石显示出更长的催化寿命(至少增加 27.6%)和更高的(C2 H 4 +C 3 H 6 ) 在甲醇制烯烃 (MTO) 反应过程中比传统水热法合成的纯 CHA 沸石提高 2.5%。以相同方式使用二次回收母液合成的沸石在 MTO 工艺中也表现出相当的催化性能,再次验证了我们的方法回收母液的可行性。在这项工作中开发的可持续合成路线应适用于各种沸石的工业生产。

更新日期:2022-08-28
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