Relationship between Lewis acid sites and carbohydrate reactivity over Sn-β catalysts†

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL
Yacine Boudjema, Antoine Brunel, Raphaël Del Cerro, Gerhard Pirngruber, Céline Chizallet and Kim Larmier
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Abstract

Sn-β is a promising Lewis acid zeolite for carbohydrate conversion. This material can be prepared either directly by hydrothermal synthesis or by a dealumination – metal incorporation sequence starting from a pre-made zeolite (post-synthesis modification). The synthesis method and the metallic precursors significantly influence the formation of Lewis acid sites in the zeolite, which is the primary factor determining the activity of the catalyst in many reactions. We synthesized various materials through post-synthesis modifications and a hydrothermal method using three different precursors. Pyridine adsorption monitored by FTIR spectroscopy shows that Sn-β samples synthesized by solid state insertion with tin chloride as a precursor feature a concentration of Lewis acid sites proportional to the tin content (up to 1.5 wt% of tin) without forming an oxide phase. Hydrothermal synthesis leads to a sample exhibiting weaker acid sites. The catalyst yields three major products in glucose conversion: fructose, mannose, and lactic acid. The high yield of lactic acid (≈30%) indicates a faster ketose retro-aldolization compared to aldose (no C4 or C2 products detected).

Abstract Image

Sn-β催化剂上Lewis酸位点与碳水化合物反应性的关系
Sn-β是一种很有前途的用于碳水化合物转化的路易斯酸沸石。该材料既可以通过水热合成直接制备,也可以通过从预制沸石(合成后改性)开始的脱铝-金属掺入顺序制备。合成方法和金属前驱体对沸石中路易斯酸位点的形成有显著影响,这是决定许多反应中催化剂活性的主要因素。我们使用三种不同的前驱体,通过合成后修饰和水热法合成了各种材料。FTIR光谱对吡啶吸附的监测表明,以氯化锡为前驱体的固态插入法制备的Sn-β样品具有与锡含量成正比的Lewis酸位点浓度(高达1.5 wt%的锡),且未形成氧化相。水热合成导致样品表现出较弱的酸位。该催化剂在葡萄糖转化过程中产生三种主要产物:果糖、甘露糖和乳酸。乳酸的高收率(≈30%)表明与醛糖相比,酮糖的反醛化速度更快(未检测到C4或C2产物)。
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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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