Shi Ning, Zhu Tianlang, Zhang Hongyan, Huang Hongsheng, Zhou Liang, Liu Ying, Shu Riyang
School of Chemical Engineering, Guizhou Institute of Technology, Guiyang 550003, China.
Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter, School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China.
ACS Omega. 2023 Mar 14;8(12):11574-11582. doi: 10.1021/acsomega.3c00708. eCollection 2023 Mar 28.
Catalytic conversion of cellulose into the novel platform molecule 2,5-hexanedione (HXD) is regarded as one feasible approach for high-value utilization of biomass resources. Here, we reported one efficient way of one-pot conversion of cellulose into HXD with high yield of 80.3% in HO and tetrahydrofuran (THF) mixture within Al(SO) combined with Pd/C as a catalyst. In the catalytic reaction system, Al(SO) could catalyze the conversion of cellulose into 5-hydroxymethylfurfural (HMF), and Pd/C combined with Al(SO) could catalyze the hydrogenolysis of HMF into furanic intermediates such as 5-methylfurfuryl alcohol and 2,5-dimethylfuran (DMF) without causing over-hydrogenation of these furanic intermediates. These furanic intermediates were finally transformed into HXD catalyzed by Al(SO). Besides, the HO/THF ratio could significantly influence the reactivity of the hydrolytic furanic ring-opening of the furanic intermediates. The catalytic system also showed excellent performance on the conversion of other carbohydrates (glucose and sucrose) into HXD.
将纤维素催化转化为新型平台分子2,5-己二酮（HXD）被认为是生物质资源高值利用的一种可行方法。在此，我们报道了一种在Al₂(SO₄)₃与Pd/C作为催化剂的情况下，在水和四氢呋喃（THF）混合物中一锅法将纤维素高效转化为HXD的方法，产率高达80.3%。在催化反应体系中，Al₂(SO₄)₃可催化纤维素转化为5-羟甲基糠醛（HMF），而Pd/C与Al₂(SO₄)₃联合可催化HMF氢解为呋喃类中间体，如5-甲基糠醇和2,5-二甲基呋喃（DMF），且不会导致这些呋喃类中间体过度氢化。这些呋喃类中间体最终在Al₂(SO₄)₃催化下转化为HXD。此外，水/THF比例可显著影响呋喃类中间体水解开环的反应活性。该催化体系在将其他碳水化合物（葡萄糖和蔗糖）转化为HXD方面也表现出优异性能。
