Highly selective synthesis of 2-cyclopentylidenecyclopentanone via cyclopentanone self-condensation over MgAl-LDO(NO3−)

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Xue Luo, Jiahui Liu, Danhui Li, Lili Zhao and Hualiang An
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Abstract

Cyclopentanone self-condensation to 2-cyclopentylidenecyclopentanone is one of the key steps in synthesizing high-density fuels. In this study, MgAl-LDO(NO3−) catalysts, prepared via coprecipitation, demonstrated good catalytic performance. Meanwhile, Mg2Al-LDO(NO3−) catalysts with different Mg/Al ratios were explored. Characterization by XRD, NH3-TPD and CO2-TPD revealed that Mg2Al-LDO(NO3−) possessed appropriate acid–base active sites, correlating with its enhanced catalytic performance. Under optimized reaction conditions, cyclopentanone conversion reached 85.9% with 98.8% selectivity toward 2-cyclopentylidenecyclopentanone. Furthermore, the reusability of the catalyst was investigated. XRD, SEM, and N2 adsorption–desorption analyses indicated that structural changes in the Mg2Al-LDO(NO3−) catalyst led to its deactivation. GC-MS analysis of the reaction system identified the primary by-product as 2,5-dicyclopentylidenecyclopentanone. Based on these findings, a plausible reaction network is proposed.

Abstract Image

MgAl-LDO(NO3−)上环戊酮自缩合高选择性合成2-环戊基环戊酮
环戊酮自缩合制2-环戊烷环戊酮是高密度燃料合成的关键步骤之一。在本研究中,通过共沉淀法制备的MgAl-LDO(NO3−)催化剂表现出良好的催化性能。同时,对不同Mg/Al比的Mg2Al-LDO(NO3−)催化剂进行了探索。XRD、NH3-TPD和CO2-TPD表征表明,Mg2Al-LDO(NO3−)具有合适的酸碱活性位点,这与其催化性能的增强有关。在优化后的反应条件下,环戊酮的转化率为85.9%,对2-环戊烷环戊酮的选择性为98.8%。此外,还研究了催化剂的可重复使用性。XRD, SEM和N2吸附-脱附分析表明,Mg2Al-LDO(NO3−)催化剂的结构变化导致其失活。气相色谱-质谱分析鉴定该反应体系的主要副产物为2,5-双环戊烷环戊酮。基于这些发现,我们提出了一个合理的反应网络。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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