含路易斯酸的Ni-Al层状双氢氧化物催化糠醛缩醛化反应动力学及机理

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Progress in Reaction Kinetics and Mechanism Pub Date : 2018-03-01 DOI:10.3184/146867817X15066861009956
Yali Du, Yalin Feng, Chunlei Zou, Xu Wu, Wei Huang
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引用次数: 7

摘要

采用六亚甲基四胺水解法制备了硝酸态Ni-Al层状双氢氧化物(Ni-Al - no3 - ldh)和碳酸盐态Ni-Al - co3 - ldh。对Ni-Al-CO3-LDH的催化性能进行了研究,结果表明Ni-Al-NO3-LDH在糠醛缩醛制糠醛二乙基缩醛反应中具有良好的催化活性和可重复使用性。表征和分析表明,Ni-Al-NO3-LDH中Lewis酸位点的出现是其具有优异催化性能的原因。得到的动力学参数证实该反应为一级反应,表观活化能为36.28 kJ mol−1,与理论结果38.57 kJ mol−1基本一致。此外,除了典型的Brønsted酸催化机理外,还从理论上探讨了一种可能的Lewis酸催化机理。
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Kinetics and Mechanism of Acetalisation of Furfural to Furfural Diethyl Acetal with Ni–Al Layered Double Hydroxides Containing Lewis Acid Sites
The nitrate form of Ni–Al layered double hydroxide (denoted as Ni–Al–NO3-LDH) and the corresponding carbonate form (denoted as Ni–Al–CO3-LDH) were tunably fabricated by the hexamethylenetetramine hydrolysis method. A catalytic behaviour investigation proved Ni–Al–CO3-LDH to be an ineffective catalyst, while for Ni–Al–NO3-LDH excellent catalytic activity and reusability were obtained, in the acetalisation of furfural to furfural diethyl acetal. Characterisation and analysis revealed that the appearance of Lewis acid sites in Ni–Al–NO3-LDH was responsible for its excellent catalytic performance. The acquired kinetic parameters confirmed that this reaction was a first-order process and the apparent activation energy was 36.28 kJ mol−1, which is in reasonable agreement with the theoretical result of 38.57 kJ mol−1. Additionally, apart from the typical Brønsted acid catalytic mechanism, a possible Lewis acid catalytic mechanism was probed theoretically.
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来源期刊
CiteScore
2.10
自引率
0.00%
发文量
5
审稿时长
2.3 months
期刊介绍: The journal covers the fields of kinetics and mechanisms of chemical processes in the gas phase and solution of both simple and complex systems.
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