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Mesoporous tantalum phosphates: preparation, acidity and catalytic performance for xylose dehydration to produce furfural

机译:介孔磷酸钽:木糖脱水制备糠醛的制备,酸度和催化性能

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摘要

Mesoporous tantalum phosphates (TaOPO4-m) with varying P/Ta molar ratios (m = 0.41-0.89) were prepared, comprehensively characterized by ICP-AES, N-2 physisorption, small-angle XRD, TEM, Raman, FT-IR, NH3-TPD and IR of pyridine adsorption and employed to catalyze the dehydration of xylose to produce furfural in a biphasic batch reactor. The physicochemical properties of these TaOPO4-m samples were affected significantly by variation of m. More ordered mesopores were formed in the sample with a higher m. On the other hand, the density of acidity decreased but the ratio of Bronsted acidity to Lewis acidity (B/L) increased with the increase in m. TaOPO4-0.84, which showed adequate mesoporosity and a high B/L ratio, was identified as the best performing catalyst among these TaOPO4-m catalysts in terms of high furfural selectivity (ca. 72 mol%). Correlating the catalyst performance with its acid property showed that the xylose consumption rate decreased with the increasing B/L ratio, while furfural selectivity showed a volcano-type dependence on the B/L ratio. Besides, the huge decrease in the furfural selectivity after poisoning the Bronsted acid sites by adding 2,6-dimethyl pyridine revealed a kind of Bronsted acid catalysis for selective furfural production.
机译:制备了具有不同P / Ta摩尔比(m = 0.41-0.89)的介孔磷酸钽(TaOPO4-m),并通过ICP-AES,N-2物理吸附,小角XRD,TEM,拉曼,FT-IR, NH3-TPD和IR吸附在吡啶中,并用于在两相间歇式反应器中催化木糖脱水以生产糠醛。这些TaOPO4-m样品的理化性质受m的变化影响很大。样品中具有更高m的有序中孔形成更多。另一方面,酸度密度降低,但布朗斯台德酸度与路易斯酸度之比(B / L)随m的增加而增加。显示出足够的介孔性和高的B / L比的TaOPO4-0.84被认为是在这些TaOPO4-m催化剂中表现出最高的糠醛选择性(约72mol%)的最佳催化剂。将催化剂性能与其酸性质相关联表明,木糖消耗速率随着B / L比的增加而降低,而糠醛选择性显示出火山类型对B / L比的依赖性。此外,通过添加2,6-二甲基吡啶使布朗斯台德酸位中毒后糠醛选择性大大降低,这表明布朗斯台德酸催化选择性糠醛生产。

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