POMs纳米空心球合成及催化纤维素制备HMF性能

Synthesis of POMs Nanohollow Spheres and Catalytic Performance in Preparation of HMF from Cellulose

5-羟甲基糠醛(HMF)是一种关键的生物基化学品,广泛应用于燃料、塑料和医药等领域。从纤维素出发,高效、绿色制备HMF是一项巨大挑战。采用天然蜂蜡作为相变模板,利用软模板法构建一类纳米空心球状多金属氧酸盐(POMs)催化剂(CTA)_(n)H_(3-n)PW_(12)O_(40)(n=0~3,简称(CTA)_(n)H_(3-n)PW),独特的BrΦnsted性、空心球结构及吸附性保证了从纤维素出发高效水解制备5-HMF。(CTA)H_(2)PW空心球催化剂实现了纤维素转化率100%和HMF产率62.3%,在天然纤维素棉花、人工提取纤维素槿纤及落叶松综纤维素几种不同来源的纤维素中也表现出广泛的原料适用性。重复使用10次后,催化剂活性没有明显下降,表现出优异的非均相性和热稳定性。

5-Hydroxymethylfurfural(HMF),an important bio-based chemical,is widely used in fuels,plastics and pharmaceuticals.Efficient and green production of HMF from cellulose remains a significant challenge.A series of hollow-sphere polyoxometalate(POMs)catalysts,(CTA)_(n)H_(3-n)PW_(12)O_(40)(n=0~3,abbreviated as(CTA)_(n)H_(3-n)PW),were successfully synthesized by using natural beeswax as a phase-change template in conjunction with a soft-template method.The unique BrΦnsted acidity,hollow-sphere structure and adsorption properties of the catalyst ensure efficient hydrolysis of cellulose to produce 5-HMF.(CTA)H_(2)PW hollow-sphere catalyst achieve a cellulose conversion rate of 100%and HMF yield of 62.3%.This catalyst also demonstrated broad applicability to various raw materials,including natural cotton cellulose,artificially extracted hibiscus cellulose and larch hemicellulose.After ten cycles of reuse,the catalyst’s activity do not significantly decline,demonstrating excellent heterogeneity and thermal stability.