Controllable transformation of biomass-derived diols over an ammonia-modified H-Beta zeolite

被引:0
作者
Ai, Shuo [1 ]
Huang, Zhenhua [1 ]
Feng, Zhenhua [1 ]
Gao, Kaili [1 ]
Liu, Linghui [1 ]
机构
[1] Guangxi Univ Sci & Technol, Coll Biol & Chem Engn, Liuzhou 545006, Peoples R China
基金
中国国家自然科学基金;
关键词
ETHYLENE-GLYCOL; HYDROGENOLYSIS; CATALYSTS;
D O I
10.1039/d4nj02043j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
For the controllable transformation of C3-6 diols in ethylene glycol (EG), a H-Beta zeolite catalyst was modified with NH3via incomplete desorption. 60.8% of acid sites on the zeolite were deactivated, but the ratio of strong acid sites was obviously increased. With 1,2-pentanediol (PDO) as a representative large-carbon-number diol, the undesirable acetalization and oligomerization reactions of EG were suppressed in the EG-PDO reaction system over the modified catalyst due to their dependency on total acid sites. NH3-TPD and FTIR results proved that Lewis acid sites on the modified zeolite were eliminated after modification, resulting in the suppression of acetalization and oligomerization reactions. In contrast, a portion of strong Br & oslash;nsted acid sites still remained, ensuring the catalytic transformation of PDO. Only 8.2% of EG was consumed after 8 h reaction, and the conversion of PDO could reach 84.3%. The loading of NH3 on the surface of zeolite pores led to diffusion resistance, slightly decreasing the reaction rate of PDO without affecting the reaction selectivity. The catalytic reactions of other C3-6 diols in EG followed similar principles, and the selectivity to aldehydes or ketone was improved over this modified catalyst. Non-diol biomass hydrogenation products such as glycerol had a negative influence on the selectivity, so these components should be isolated before the reactions. This catalyst could be reused at least 5 times, and the conversion of PDO slightly decreased. This work sheds light on the relationships between the acid properties of the catalyst and different reactions of diols. For the controllable transformation of C3-6 diols in ethylene glycol (EG), a H-Beta zeolite catalyst was modified with NH3via incomplete desorption.
引用
收藏
页码:13186 / 13195
页数:10
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