Homocondensation of Acetone over Cation-Exchanged Granulated Hierarchical Yh Zeolites

IF 1.1 4区 工程技术 Q3 CHEMISTRY, ORGANIC
V. Yu. Kirsanov, L. F. Korzhova, S. G. Karchevsky, A. N. Khazipova, B. I. Kutepov, N. G. Grigor’eva
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Abstract

The catalytic performance (activity and selectivity) of a FAU-type hierarchical NaYh zeolite, as well as of a series of modified samples, was investigated in the homocondensation of acetone. The modified samples were prepared from NaYh by ion exchange of Na+ for cations of alkali (Li+, K+), alkaline-earth (Ca2+, Mg2+), transition (Co2+, Ni2+), and rare-earth (La3+) metals, as well as by decationation (H-NaYh, HYh). The predominantly acidic zeolites (Ca-NaYh, Mg-NaYh, Co-NaYh, Ni-NaYh, La-NaYh, H-NaYh, and HYh) promoted the formation of acetic acid and mesitylene even at 250°C. The zeolites that contained alkali metal cations (Na+, Li+, and K+) exhibited activity only when the temperature was elevated. Starting from 350°C, NaYh and Li-NaYh promoted the formation of acetic acid. In contrast, the performance of K-NaYh under heating was characterized by the absence of acetic acid formation and a smooth increase in the selectivity towards isophorone (up to 23%) and mesitylene (up to 18%). Over the range of 400–450°C, in the presence of K-NaYh, secondary isophorone transformations were intensified, resulting in the formation of 3,5-xylenol as the main product with a selectivity of 32%.

Abstract Image

丙酮在阳离子交换的粒状分级Yh沸石上的同缩合反应
研究了fau型层次型NaYh分子筛及其改性样品在丙酮均缩合反应中的催化性能(活性和选择性)。用Na+离子交换碱离子(Li+, K+)、碱土离子(Ca2+, Mg2+)、过渡态离子(Co2+, Ni2+)和稀土离子(La3+),并采用H-NaYh, HYh进行了修饰。酸性沸石(Ca-NaYh、Mg-NaYh、Co-NaYh、Ni-NaYh、La-NaYh、H-NaYh和HYh)在250℃时也能促进乙酸和三甲基甲苯的生成。含有碱金属阳离子(Na+、Li+和K+)的沸石只有在温度升高时才表现出活性。从350°C开始,NaYh和Li-NaYh促进了乙酸的形成。相比之下,K-NaYh在加热条件下的性能表现为不生成乙酸,对异佛尔酮(高达23%)和三甲苯(高达18%)的选择性平稳增加。在400 ~ 450℃范围内,在K-NaYh存在下,异虫酮的二次转化增强,生成的主要产物为3,5-二甲酚,选择性为32%。
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来源期刊
Petroleum Chemistry
Petroleum Chemistry 工程技术-工程:化工
CiteScore
2.50
自引率
21.40%
发文量
102
审稿时长
6-12 weeks
期刊介绍: Petroleum Chemistry (Neftekhimiya), founded in 1961, offers original papers on and reviews of theoretical and experimental studies concerned with current problems of petroleum chemistry and processing such as chemical composition of crude oils and natural gas liquids; petroleum refining (cracking, hydrocracking, and catalytic reforming); catalysts for petrochemical processes (hydrogenation, isomerization, oxidation, hydroformylation, etc.); activation and catalytic transformation of hydrocarbons and other components of petroleum, natural gas, and other complex organic mixtures; new petrochemicals including lubricants and additives; environmental problems; and information on scientific meetings relevant to these areas. Petroleum Chemistry publishes articles on these topics from members of the scientific community of the former Soviet Union.
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