Synthesis of monolithic SSZ-13 zeolite by dry-gel conversion method

doi:10.11949/j.issn.0438-1157.20161381

Abstract

Abstract:

In this work, monolithic SSZ-13 zeolite was synthesized using dry-gel conversion method. The influences of the gel composition and crystallization conditions on the crystallization of SSZ-13 zeolite were investigated. The as-synthesized product was characterized by X-ray diffraction (XRD), X-ray fluorescence (XRF),thermo gravimetric-differential thermal analysis (TG-DTA, scanning electron microscope(SEM), NH₃ temperature-programmed desorption(NH₃-TPD, Nuclear Magnetic Resonance (NMR). The roles of N,N,N-trimethyl-1-adamantanammonium (TMADa⁺) and choline chloridein crystallization reaction were discussed. According to the result, the monolithic SSZ-13 zeolite has typical accumulated mesopores, larger surface area and better thermal stability in air. The results in FT-IR and NMR spectra show that choline chloride could act as a secondary structure-directing agent and fill in the pores of zeolite, which significantly reduced the amount of TMADa⁺. It was confirmed that Choline Chloride favors accelerating zeolite nucleation, shortening the crystallization time, and improving crystallinity of the as-synthesized product.

Key words: dry-gel conversion, monolithic, SSZ-13, zeolite, crystallization, choline chloride, structural-directing, nucleation

摘要：

采用干胶转化法合成了整体式SSZ-13分子筛，先成型后晶化，系统地考察了物料配比及晶化条件对合成结果的影响，通过X射线衍射（XRD）、X射线荧光（XRF）、热重-差热分析仪（TG-DTA）、扫描电子显微镜（SEM）、氨气的程序升温吸附-脱附（NH₃-TPD）、傅里叶红外光谱仪（FI-IR）、液体核磁共振谱（NMR）对产物进行表征分析，并讨论了混合模板剂N，N，N-三甲基-1-金刚烷氢氧化铵和氯化胆碱在晶化过程中起的作用。结果表明，合成的整体式SSZ-13分子筛具有典型的介孔堆积孔、较大的比表面积，在空气中热稳定性良好。氯化胆碱加速了分子筛晶化，缩短了晶化时间，提高产物的结晶度，明显降低了N，N，N-三甲基-1-金刚烷氢氧化铵的使用量，起到了辅助结构导向的作用，且混合模板剂均填充产物孔道。

关键词: 干胶转化, 整体式, SSZ-13, 分子筛, 结晶, 氯化胆碱, 结构导向, 成核

CLC Number:

TQ426.94

FENG Qing, PEI Renyan, LIU Hongguang, YU Haibin, ZHANG Lijuan, ZHANG Yaori. Synthesis of monolithic SSZ-13 zeolite by dry-gel conversion method[J]. CIESC Journal, 2017, 68(3): 1231-1238.

冯晴, 裴仁彦, 刘红光, 于海斌, 张丽娟, 张耀日. 干胶转化法合成整体式SSZ-13分子筛[J]. 化工学报, 2017, 68(3): 1231-1238.

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