Synthesis of hierarchical ZSM-12 nanolayers for levulinic acid esterification with ethanol to ethyl levulinate.
Synthesis of hierarchical ZSM-12 nanolayers for levulinic acid esterification with ethanol to ethyl levulinate.
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DOI：
10.1039/c9ra03213d
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发表时间：
2019-06-10
期刊：
影响因子：
3.9
通讯作者：
Wattanakit, Chularat
中科院分区：
文献类型：
--
作者：
Dugkhuntod, Pannida;Imyen, Thidarat;Wannapakdee, Wannaruedee;Yutthalekha, Thittaya;Salakhum, Saros;Wattanakit, Chularat
以二甲基十八烷基[3-（三甲氧基硅基）丙基]氯化铵（TPOAC）为第二有机结构导向剂（OSDA），通过一锅法水热合成了分级ZSM-12纳米层。采用XRD、SEM、TEM、N2物理吸附、NH3-TPD等手段对合成的ZSM-12进行了表征。这清楚地表明TPOAC含量和结晶时间是形成纳米层结构的关键参数。这种结构的存在通过在纳米层之间产生间隙中孔，最终导致提高外表面积和中孔体积，并随后促进沸石骨架内的分子扩散，显著改善了ZSM-12的中孔性。为了说明其作为非均相催化剂的优点，将分级ZSM-12纳米层应用于乙酰丙酸与乙醇酯化成乙酰丙酸乙酯的催化应用中。有趣的是，分级ZSM-12纳米层在乙酰丙酸转化率（78.5%）和乙酰丙酸乙酯选择性（98.7%）方面与分级沸石纳米片的其他框架（例如ZSM-5和FAU）相比表现出催化活性的改善。本文报道的实施例证明了通过双模板法合成具有分级纳米层结构的一维孔沸石的有效方法，并且还为沸石的不同分级多孔系统在大分子反应中的应用开辟了前景，例如在乙酰丙酸与乙醇酯化的情况下。采用双模板法合成了多级结构的ZSM-12纳米分子筛，并将其作为乙酰丙酸酯化反应的高效催化剂。
Hierarchical ZSM-12 nanolayers have been successfully synthesized via a one-pot hydrothermal process using dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (TPOAC) as a secondary organic structure-directing agent (OSDA). The as-synthesized ZSM-12 samples were characterized by means of XRD, SEM, TEM, N2 physisorption, and NH3-TPD. This clearly demonstrates that the TPOAC content and the crystallization time are crucial parameters for the formation of nanolayered structures. The presence of such a structure significantly improves the mesoporosity of ZSM-12 by generating interstitial mesopores between nanolayers, eventually resulting in enhancing external surface areas and mesopore volumes, and subsequently promoting the molecular diffusion inside a zeolite framework. To illustrate its advantages as a heterogeneous catalyst, hierarchical ZSM-12 nanolayers were applied in the catalytic application of an esterification of levulinic acid with ethanol to ethyl levulinate. Interestingly, hierarchical ZSM-12 nanolayers exhibit an improvement of catalytic activity in terms of levulinic acid conversion (78.5%) and ethyl levulinate selectivity (98.7%) compared with other frameworks of hierarchical zeolite nanosheets, such as ZSM-5 and FAU. The example reported herein demonstrates an efficient way to synthesize a unidimensional pore zeolite with hierarchical nanolayered structure via a dual template method and also opens up perspectives for the application of different hierarchical porous systems of zeolites in the bulky-molecule reactions such as in the case of levulinic acid esterification with ethanol. Hierarchical ZSM-12 nanolayers were successfully synthesized via a dual template approach as an efficient catalyst for levulinic acid esterification.
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