Synthesis of hierarchically porous tantalum phosphate catalysts by a sol–gel method for transformation of glucose to 5-hydroxymethylfurfural

IF 4.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2025-01-21 Epub Date: 2025-01-17 DOI:10.1039/d4cy01112k
Kai Huang , Taoli Huhe , Haichao Liu , Da-Ming Gao , Yao Zhai
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Abstract

A hierarchically porous and highly effective tantalum phosphate (TaP) solid acidic catalyst was synthesized using a sol–gel method accompanied by phase separation for converting glucose to 5-hydroxymethylfurfural (HMF). The TaP sample formed the TaPO5 phase after calcining at 600 °C (TaP-600) for 4 hours with a surface area of ca. 103 m2 g−1 and an acidity of ca. 0.18 mmolNH3 g−1. The TaP-600 sample had a co-continuous macroporous structure with a regular and orderly pore arrangement, which was conducive to the diffusion of reactants and products, thereby reducing side reactions. The TaP-600 sample can afford an HMF yield of 25.6% by treating with 1.0 wt% glucose at 170 °C in pure water. Using a water–DMSO homogeneous system or a water/MIBK biphasic reaction system can protect HMF from further decomposition, obtaining a HMF yield of 63.8% and 67.1% (mol mol−1), respectively. The TaP-600 sample also showed high catalytic performance at high glucose concentration in the water/MIBK system, e.g. the HMF yields reached 27.5% and 23.7% at glucose concentrations of 15.0 wt% and 20.0 wt%, respectively. The productivity of HMF reached 6.6 × 10−2 mol h−1 kgsolution−1 at an initial glucose concentration of 20.0 wt% in the water/MIBK biphasic system with a catalyst loading (weight ratio of catalyst to glucose) of 10.0 wt%. The TaP-600 sample can retain most of its activity after three catalytic cycles giving an HMF yield of 17.9%. These results demonstrate the significant potential of TaP for industrial-scale HMF production.

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溶胶-凝胶法制备葡萄糖转化为5-羟甲基糠醛的分级多孔磷酸钽催化剂
采用溶胶-凝胶相分离法制备了一种结构多孔、高效的磷酸钽(TaP)固体酸性催化剂,用于将葡萄糖转化为5-羟甲基糠醛(HMF)。TaP样品在600℃(TaP-600)煅烧4小时后形成TaPO5相,其表面积约为103 m2 g−1,酸度约为0.18 mmolNH3 g−1。TaP-600样品具有共连续的大孔结构,孔隙排列规则有序,有利于反应物和生成物的扩散,从而减少副反应。TaP-600样品在170°C的纯水中用1.0 wt%的葡萄糖处理,HMF产率可达25.6%。采用水- dmso均相体系或水/MIBK双相反应体系可以防止HMF进一步分解,HMF产率分别为63.8%和67.1% (mol mol−1)。TaP-600样品在高葡萄糖浓度的水/MIBK体系中也表现出较高的催化性能,例如,在葡萄糖浓度为15.0 wt%和20.0 wt%时,HMF的产率分别达到27.5%和23.7%。在初始葡萄糖浓度为20.0 wt%、催化剂负载(催化剂与葡萄糖的重量比)为10.0 wt%的水/MIBK双相体系中,HMF的产率达到6.6 × 10−2 mol h−1 kgsolution−1。TaP-600样品在三次催化循环后仍能保持大部分活性,HMF收率为17.9%。这些结果表明TaP在工业规模生产HMF方面具有巨大的潜力。
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文献相关原料
公司名称
产品信息
麦克林
Methyl isobutyl ketone
麦克林
Methanol
麦克林
Anhydrous ethanol
麦克林
Fructose
麦克林
Glucose
麦克林
5-hydroxymethylfurfural
来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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