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Au/γ-Al2O3 catalysts for glycerol oxidation: the effect of support acidity and gold particle size

机译:用于甘油氧化的Au /γ-Al2O3催化剂:载体酸性和金粒径的影响

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摘要

In this study, the effect of gold particle size and surface acidity were investigated in the partial oxidation of glycerol, particularly towards the formation of lactic acid over gold catalysts supported on acidified γ-Al2O3. Alumina-supported gold catalysts were prepared at an optimal pH of approximately 7.0 and tested for the partial oxidation of glycerol. To acidify the catalyst samples, M0O3 or WO3 monolayer was introduced onto the alumina support before gold was deposited. It was observed that under the reaction conditions employed, small gold nanoparticles (ca 4 nm) showed a tendency towards zeroth order kinetics for the oxidation of glycerol. However, bigger gold nanoparticles (ca 20 nm) were inclined towards first order kinetics. It was also established that the nature of the reducing agent affected the size and morphology of the supported gold nanoparticles on γ-alumina and consequently the product spectrum. Catalysts with smaller gold nanoparticles formed predominantly C-3 compounds (glyceric, tartronic and lactic acids) while those with bigger gold nanoparticles formed predominantly C-1 compound (formic acid). Increased Lewis acidity was also found to play a positive role in the formation of lactic acid over γ-alumina-supported gold catalyst.
机译:在这项研究中,研究了金的粒径和表面酸度对甘油部分氧化的影响,特别是对在酸化的γ-Al2O3上负载的金催化剂上形成乳酸的影响。在约7.0的最佳pH下制备了氧化铝负载的金催化剂,并测试了甘油的部分氧化。为了酸化催化剂样品,在沉积金之前将MO 3或WO 3单层引入到氧化铝载体上。观察到在所采用的反应条件下,小的金纳米颗粒(约4 nm)显示出甘油氧化趋于零级动力学的趋势。但是,较大的金纳米粒子(约20 nm)倾向于一级动力学。还确定还原剂的性质影响γ-氧化铝上负载的金纳米颗粒的尺寸和形态,并因此影响产物光谱。具有较小金纳米颗粒的催化剂主要形成C-3化合物(甘油,酒石酸和乳酸),而具有较大金纳米颗粒的催化剂主要形成C-1化合物(甲酸)。还发现路易斯酸的增加在γ-氧化铝负载的金催化剂上对乳酸的形成起积极作用。

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