Hierarchical NaY Zeolites for Lactic Acid Dehydration to Acrylic Acid

被引:46
作者
Lari, Giacomo M. [1 ]
Puertolas, Begona [1 ]
Frei, Matthias S. [1 ]
Mondelli, Cecilia [1 ]
Perez-Ramirez, Javier [1 ]
机构
[1] ETH, Inst Chem & Bioengn, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
基金
瑞士国家科学基金会;
关键词
acidity; basicity; biomass; dehydration; zeolites; NA-23; NMR-SPECTROSCOPY; BASE CATALYSTS; GLYCEROL; SITES; CHEMOCATALYSIS; PHOSPHATES; CONVERSION; DESIGN; BIO;
D O I
10.1002/cctc.201600102
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The industrial viability of heterogeneous catalysts for the gas-phase conversion of lactic acid to acrylic acid will strongly depend on their selectivity and durability. Here, we initially screened various aluminum-rich zeolites confirming that NaY is the most efficient catalyst for this reaction. This material was modified by sequential dealumination and alkaline treatment attaining a solid featuring a hierarchical distribution of micro- and mesopores, reduced Lewis acidity, and increased basicity owing to the presence of well-dispersed sodium ions interacting with external siloxy groups, as evidenced by in-depth characterization. These properties were crucial for determining higher selectivity (75%) and minimizing the activity loss in a 6h run. Remarkably, the catalyst gained in selectivity and stability upon reuse in consecutive cycles. This was ascribed to the depletion of the stronger basic sites and the clustering of sodium into oxidic particles upon the intermediate calcination.
引用
收藏
页码:1507 / 1514
页数:8
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