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Improved chemoselective hydrogenation of crotonaldehyde over bimetallic AuAg/SBA-15 catalyst

机译:在双金属AuAg / SBA-15催化剂上改进巴豆醛的化学选择性加氢

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摘要

Bimetallic AuAg/SBA-15 catalysts were disclosed to efficiently catalyze vapor-phase chemoselective hydrogenation of crotonaldehyde (CRAL) with improved hydrogenation rate and selectivity to crotonyl alcohol (CROL). The CRAL hydrogenation rate and product distribution were remarkably influenced by reaction parameters such as the reaction pressure and CRAL/hydrogen ratio. Ag decoration on Au/SBA-15 effectively stabilized bimetallic AuAg nano-alloy particles in small size and promoted the catalytic stability. In situ FT-IR investigation revealed that unusual C2M2 di-sigma bonded CRAL surface species with reinforced symmetric delta(CH3) IR band under the "metal-surface selection rule" (MSSR) were formed on bimetallic AuAg/SBA-15. The stronger CRAL chemisorption on bimetallic AuAg/SBA-15 surfaces than on monometallic Au/SBA-15 was possibly due to the relatively strong ligating of C=O bond on Ag active sites and the enhancement of the co-adsorption of the conjugated double bonds of CRAL. Synergistic interaction between Au and Ag active sites for the activation of H-H, C=C and C=O bond may be the origin of positive effect of Ag decoration on Au/SBA-15. (C) 2015 Elsevier Inc. All rights reserved.
机译:公开了双金属AuAg / SBA-15催化剂,以改进的氢化速率和对巴豆基醇(CROL)的选择性,有效地催化巴豆醛(CRAL)的气相化学选择性氢化。反应压力,CRAL /氢比等反应参数对CRAL的氢化率和产物分布有显着影响。 Au / SBA-15上的Ag装饰有效地稳定了小尺寸的双金属AuAg纳米合金颗粒,并提高了催化稳定性。原位FT-IR研究表明,在双金属AuAg / SBA-15上形成了具有“对称金属-表面选择规则”(MSSR)且具有增强的对称δ(CH3)IR谱带的不寻常的C2M2双σ键合的CRAL表面物质。双金属AuAg / SBA-15表面上的CRAL化学吸附比单金属Au / SBA-15上的CRAL化学吸附更强,这可能是由于C = O键在Ag活性位点上的连接相对较强,以及共轭双键的共吸附作用增强CRAL。 Au和Ag活性位点之间的H-H,C = C和C = O键激活协同相互作用可能是Ag装饰对Au / SBA-15产生积极作用的起源。 (C)2015 Elsevier Inc.保留所有权利。

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