Journal of Catalysis ( IF 6.5 ) Pub Date : 2019-06-04 , DOI: 10.1016/j.jcat.2019.05.020 Hongwei Zhang , Weijia Yang , Irwan Iskandar Roslan , Stephan Jaenicke , Gaik-Khuan Chuah
A highly efficient catalyst system was developed for the one-pot transformation of furfural to γ-valerolactone (GVL) in an open system. The cascade of two Meerwein Ponndorf Verley (MPV) reductions, ring-opening and esterification reactions was catalyzed by a physical mixture of Zr- and Al-HY zeolites where the proportion and strength of Lewis and Brønsted acid sites could be independently optimized. The excellent activity of Zr-HY zeolites for the MPV reduction of furfural and levulinate ester with 2-pentanol as hydrogen donor was attributed to the larger pore size of HY-zeolites and stronger Lewis acidic sites compared to Zr-Beta. Al-HY zeolites were more effective as Brønsted acid than Al-Beta because they converted furfuryl ether to levulinate ester rather than to β-angelica lactone. The dual catalytic system comprising Zr-HY (Si/Zr 20) and Al-HY (Si/Al 6) exhibited remarkably high catalytic activity with GVL yields of 85% after only 5 h at 120 °C.
中文翻译:
Zr-HY和Al-HY分子筛组合催化剂用于生物质糠醛一锅级联转化为γ-戊内酯
开发了一种高效的催化剂体系,用于在开放系统中将糠醛一锅转化为γ-戊内酯(GVL)。Meerwein Ponndorf Verley(MPV)还原,开环和酯化反应的级联反应由Zr-和Al-HY沸石的物理混合物催化,其中Lewis和Brønsted酸位的比例和强度可以独立优化。Zr-HY沸石以2-戊醇作为氢供体,对糠醛和乙酰丙酸酯的MPV还原具有优异的活性,这归因于与Zr-Beta相比,HY沸石的孔径更大,路易斯酸位点更强。Al-HY沸石作为布朗斯台德酸比Al-Beta更有效,因为它们将糠基醚转化为乙酰丙酸酯而不是β-当归内酯。包含Zr-HY(Si / Zr 20)和Al-HY(Si / Al 6)的双重催化体系在120°C下仅运行5小时后,催化活性就非常显着,GVL收率达85%。