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煅烧温度对镁铝层状双氢氧化物(LDH)作为乙醇氧化脱氢制乙醛的潜在催化剂的影响

Effect of Calcination Temperature on Mg-Al Layered Double Hydroxides (LDH) as Promising Catalysts in Oxidative Dehydrogenation of Ethanol to Acetaldehyde.

作者信息

Pinthong Piriya, Praserthdam Piyasan, Jongsomjit Bunjerd

机构信息

Center of Excellence on Catalysis and Catalytic Reaction Engineering, Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University.

出版信息

J Oleo Sci. 2019 Jan 1;68(1):95-102. doi: 10.5650/jos.ess18177. Epub 2018 Dec 12.

Abstract

Oxidative dehydrogenation of ethanol to acetaldehyde over Mg-Al layered double hydroxides (LDH) and their differently calcined derivative catalysts was investigated in this study. The Mg-Al catalysts were synthesized via co-precipitation method and calcined at different temperatures at 450°C, 600°C and 900°C. It revealed that the calcination temperature affected the physicochemical properties and the catalytic activity of these catalysts toward the oxidative dehydrogenation of ethanol. It was found that ethanol conversion increased with increasing reaction temperature from 200 to 400°C, whereas acetaldehyde selectivity decreased. At low reaction temperature (200-300°C), the non-calcined catalyst (Mg-Al-000) showed the highest ethanol conversion, which can be attributed to the hydroxyl groups on surface having acetaldehyde as a major product. The calcination process led to formation of mixed oxide phase in Mg-Al catalysts as proven by the XRD and FT-IR results. The catalyst calcined at 450°C (Mg-Al-450) exhibited the highest basicity as measured by the CO-TPD with ethanol conversion of 45.8% and acetaldehyde yield of 29.7% at 350°C.

摘要

本研究考察了乙醇在镁铝层状双氢氧化物(LDH)及其不同煅烧衍生催化剂上氧化脱氢制乙醛的反应。通过共沉淀法合成了镁铝催化剂,并在450°C、600°C和900°C的不同温度下进行煅烧。结果表明,煅烧温度影响了这些催化剂的物理化学性质以及对乙醇氧化脱氢的催化活性。研究发现,随着反应温度从200°C升高到400°C,乙醇转化率增加,而乙醛选择性降低。在低反应温度(200 - 300°C)下,未煅烧的催化剂(Mg - Al - 000)表现出最高的乙醇转化率,这可归因于表面的羟基以乙醛为主要产物。XRD和FT - IR结果证明,煅烧过程导致镁铝催化剂中形成混合氧化物相。通过CO - TPD测定,在450°C煅烧的催化剂(Mg - Al - 450)表现出最高的碱度,在350°C时乙醇转化率为45.8%,乙醛产率为29.7%。

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