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首页> 外文期刊>Catalysis science & technology >The design and catalytic performance of molybdenum active sites on an MCM-41 framework for the aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran
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The design and catalytic performance of molybdenum active sites on an MCM-41 framework for the aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran

机译：钼的设计和催化性能活跃的站点MCM-41框架有氧氧化5-hydroxymethylfurfural2,5-diformylfuran

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摘要

Mo-Containing catalysts exhibit good catalytic performance toward the selective oxidation of platform chemicals from biomass. However, for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF), the development of an environmentally-friendly and promising catalytic system remains a significant challenge to date. In the present study, on the pore surface of MCM-41, two kinds of active sites, which are, -(SiO)(2)Mo(O)(2) ([Mo-4]) and -(SiO)(3)Mo(OH)(O) ([Mo-5]), have been theoretically designed, over which the catalytic mechanisms for the aerobic oxidation of HMF to DFF have been theoretically examined, combining the hybrid quantum mechanics and molecular mechanics calculations. Over both [Mo-4] and [Mo-5] active sites, the oxidative reaction includes two main reaction steps, the O-H and C-H bond cleavages of HMF, in which the crucial reaction step is associated with the C-H bond cleavage of the CH2 group of the first HMF. Over the -(O)(4)-Mo?O active site on the Keggin heteropolyacid ([Mo-HPA]), [Mo-4] and [Mo-5] active sites, the Mo?O group is responsible for the O-H bond activation in the HMF moiety, and the Mo-OH group is in charge of the C-H bond activation in the HMF moiety, both of which take a synergic catalytic effect. The catalytic activity decreases as [Mo-5] [Mo-4] [Mo-HPA]. Based on the activation strain analysis, the lowering activation energy stems mainly from the lowering activation strain of the active site, which correlates positively with the corresponding HOMO-LUMO gap. These findings provide deep insight for the rational design of a recyclable catalyst to activate both C-H and O-H bonds at low temperatures, especially for some typical platform molecules from biomass.
机译：Mo-Containing催化剂具有良好的催化的选择性氧化性能平台从生物质化学品。有氧氧化5-hydroxymethylfurfural(羟甲基糠醛)2,5-diformylfuran (DFF)的发展环保的和有前途的催化系统仍然是一个重大挑战到目前为止。MCM-41表面,两种活跃的网站,(,) - SiO(2)莫(O) (2) ([Mo-4])和理论上设计,在催化羟甲基糠醛的有氧氧化的机制DFF已经从理论上研究,结合混合量子力学和分子力学计算。(Mo-5)活跃的网站,氧化反应包括两个主要的反应步骤,地和碳氢键债券分裂的羟甲基糠醛,至关重要反应步骤是与碳氢键相关联乳沟CH2集团的第一个羟甲基糠醛。——(O) (4) (?活跃的网站,莫?羟甲基糠醛的键激活地一部分,碳氢键的Mo-OH集团负责激活羟甲基糠醛的一部分,这两个协同催化效应。活动减少(Mo-5)比;[Mo-HPA]。分析,降低活化能茎主要从降低激活的应变积极与相关活性部位相应HOMO-LUMO差距。提供的设计合理的深刻理解可回收的催化剂活化碳氢键和地债券在低温下,特别是对于一些典型的平台从生物分子。

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