Effects of Synthesis Variables on SAPO-34 Crystallization Templated Using Pyridinium Supramolecule and Its Catalytic Activity in Microwave Esterification Synthesis of Propyl Levulinate

Abstract

A detailed investigation of the hydrothermal crystallization of SAPO-34 in the presence of the novel 1-propylpyridinium hydroxide ([PrPy]OH) organic structural directing agent is presented. The synthesis conditions are systematically tuned to investigate the effects of various parameters (viz. concentrations of each reactant, crystallization time, and temperature) on the nucleation and crystallization of SAPO-34. The results show that a careful variation in each of the synthesis parameters results in the formation of competing phases such as SAPO-5, SAPO-35, and SAPO-36. Pure and fully crystalline SAPO-34 can be crystallized using a precursor hydrogel of a molar ratio of 2.0 Al: 4.7 P: 0.9 Si: 6.7 [PrPy]OH: 148 H2O at 200 °C for only 19 h, which is a shorter time than that found in previous studies. The prepared SAPO-34 is also very active in the esterification of levulinic acid and 1-propanol. By using microwave heating, 91.5% conversion with 100% selectivity toward propyl levulinate is achieved within 20 min at 190 °C. Hence, the present study may open a new insight into the optimum synthesis study of other zeolites using novel pyridinium organic moieties and the opportunity of replacing conventional harmful and non-recyclable homogeneous catalysts in levulinate biofuel synthesis.

Direct evidence of time-dependent crystallization evolution of SAPO-34 and SAPO-20 zeolites directed by trimethylbenzylammonium hydroxide for microwave-assisted ethanolysis of furfuryl alcohol

“…Typically, SAPO-34 can be synthesized using diethylamine, 22 triethylamine, 23 tetraethylammonium hydroxide, 24 1-propylpyridinium hydroxide, 25 piperidine 26 or morpholine 27 as organic templates, whereas SAPO-20 can only be crystallized using trimethylamine. 28 These organic templates show different shapes, hydrophilicity and sizes, and thus demonstrate different crystallization kinetics and structure-directing ability for tailoring the pore structure of zeolites.…”