MFI Acid Catalysts with Different Crystal Sizes and Porosity for the Conversion of Furanic Compounds in Alcohol Media
MFI Acid Catalysts with Different Crystal Sizes and Porosity for the Conversion of Furanic Compounds in Alcohol Media
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DOI：
10.1002/cctc.201601236
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发表时间：
2017-07
期刊：
影响因子：
4.5
通讯作者：
Margarida M. Antunes;S. Lima;A. Fernandes;Ana L. Magalhães;Patrícia Neves;Carlos M. Silva;M. Ribeiro-M.-Ribeir
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文献类型：
--
作者：
Margarida M. Antunes;S. Lima;A. Fernandes;Ana L. Magalhães;Patrícia Neves;Carlos M. Silva;M. Ribeiro-M.-Ribeir
探索了具有MFI拓扑结构和不同晶体尺寸和孔隙率的固体酸催化剂用于在T=120-170 °C下在1-丁醇中转化碳水化合物-生物质衍生的α-当归内酯和5-（羟甲基）糠醛，以得到乙酰丙酸酯和呋喃醚。采用ZSM-5沸石合成后碱/酸处理法制备了微/介孔微晶催化剂，考察了脱硅（碱）条件对材料性能的影响。通过使用水热动态条件合成纳米晶ZSM-5样品并用作参比材料。具有不同形态、质地和酸性质的材料的催化性能的比较突出了酸和质地性质之间复杂的相互作用。通过合成后处理获得了性能最佳的催化剂（MPEG0.6）;通过催化剂回收、接触试验和废催化剂表征证实了相当好的催化稳定性。在两个反应体系中，将MPEG0.6与大孔离子交换树脂Amberlyst-15（被选为基准固体酸催化剂）进行比较。
Solid acid catalysts possessing MFI topology and different crystal sizes and porosities were explored for the conversion of carbohydrate‐biomass‐derived α‐angelica lactone and 5‐(hydroxymethyl)furfural, in 1‐butanol at T=120–170 °C, to give levulinate esters and furanic ethers. Micro/mesoporous microcrystalline catalysts were prepared by post‐synthesis base/acid treatments of ZSM‐5 zeolite; the influence of the desilication (base) conditions on the material properties was investigated. A nanocrystalline ZSM‐5 sample was synthesised by using hydrothermal, dynamic conditions and used as a reference material. A comparison of the catalytic performances of materials featuring different morphological, textural, and acid properties highlights a complex interplay between the acid and textural properties. The best‐performing catalyst (MZS0.6) was obtained by post‐synthesis‐treatment; fairly good catalytic stability was confirmed by catalyst recycling, contact tests, and characterisation of the spent catalyst. MZS0.6 was compared with the macrorecticular ion‐exchange resin Amberlyst‐15, chosen as a benchmark solid acid catalyst, in the two reaction systems.