Catalytic hydrogenation performance of 2,2,4,4-tetramethyl-1,3-cyclobutanedione with Ru/activated carbon catalyst

IF 2.1 4区 化学 Q4 CHEMISTRY, PHYSICAL
Teng Zhan, Lei Ma, Suohe Yang, Guangxiang He, Longyu Wang, Haibo Jin
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Abstract

In this study, a highly dispersed Ru/AC catalyst was prepared via an isovolumetric impregnation-chemical reduction method for the selective hydrogenation of 2,2,4,4-tetramethyl-1,3-cyclobutanedione (TMCB) to 2,2,4,4-tetramethyl-1,3-cyclobutanediol (CBDO). The catalytic performance was evaluated in a high-pressure reactor with a high substrate concentration of 9 wt% under industrially relevant conditions. The influence of key process parameters on hydrogenation efficiency was systematically investigated, and the catalyst’s stability over multiple reaction cycles was thoroughly assessed. Comprehensive characterization using XRD, BET, and TEM confirmed the atomic-level dispersion of Ru nanoparticles on the activated carbon support, with an average particle size of 0.4 nm. XPS and SEM analyses conducted before and after the reaction revealed that catalyst deactivation primarily stemmed from oxidation, leaching, and agglomeration of metallic Ru0 species, resulting in a progressive loss of active sites. The Ru/AC catalyst, under optimized reaction conditions (4 wt% Ru loading, 130 °C, 4 MPa H₂ pressure, and 1 h reaction time), afforded a CBDO yield of 99%, retaining a high yield of 90% even after 10 consecutive catalytic cycles.

Ru/活性炭催化2,2,4,4-四甲基-1,3-环丁二酮加氢的性能
本研究采用等体积浸渍-化学还原法制备了高度分散的Ru/AC催化剂,用于2,2,4,4-四甲基-1,3-环丁二酮(TMCB)选择性加氢制备2,2,4,4-四甲基-1,3-环丁二醇(CBDO)。在工业相关条件下,在高底物浓度为9 wt%的高压反应器中对催化性能进行了评估。系统研究了关键工艺参数对加氢效率的影响,全面评价了催化剂在多个反应循环中的稳定性。通过XRD、BET和TEM综合表征,证实了Ru纳米颗粒在活性炭载体上的原子级分散,平均粒径为0.4 nm。反应前后的XPS和SEM分析表明,催化剂失活主要源于金属Ru0的氧化、浸出和团聚,导致活性位点的逐渐丧失。在优化的反应条件下(4 wt% Ru负载,130°C, 4 MPa H₂压力,1 H反应时间),Ru/AC催化剂的CBDO收率为99%,即使在连续10次催化循环后仍保持90%的高收率。
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来源期刊
CiteScore
3.30
自引率
5.60%
发文量
201
审稿时长
2.8 months
期刊介绍: Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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