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Hierarchical molecular sieve-based Ce-Ru oxide for enhanced catalytic oxidation of chlorobenzene: Insight into the synergistic effect of Ce and Ru, the role of molecular sieve

分子筛 氯苯 催化作用 化学 氧化物 筛子(范畴论) 化学工程 无机化学 有机化学 数学 组合数学 工程类
作者
Chengwei Yu,Jianan Gu,Yixin Xue,Mingming Guo,Kan Li,Jinping Jia,Tonghua Sun
出处
期刊:Chemical Engineering Research & Design [Elsevier BV]
卷期号:185: 632-643 被引量:6
标识
DOI:10.1016/j.psep.2024.03.047
摘要

In this work, a series of hierarchical molecular sieve were synthesized via adjusting the ratio of Si/Al. Then, Ce and Ru were supported on the molecular sieve and the loading amount of Ru were optimized. Catalytic evaluation showed that 5Ce0.5Ru/HZ-3 with the value Si/Al ratio of 80 performed the best catalytic activity of chlorobenzene oxidation with T50 and T90 values of 238 ℃ and 278 ℃, respectively and no chlorobenzene conversion can be seen on the 5Ce/HZ-3 and HZ-3, indicating that Ru was the active sites on 5Ce0.5Ru/HZ-3 and Ce played a promoter role in chlorobenzene oxidation. Catalytic stability showed that 5Ce0.5Ru/HZ-3 can maintain the complete conversion of chlorobenzene oxidation at 300°C for 190 h and the CO2 and HCl selectivity kept around 80% and 27%, respectively, while 5Ce0.5Ru performed worse catalytic stability and no HCl was detected. Subsequently, characterization results implied that HZ-3 with the Si/Al ratio of 80 had the biggest mesoporous volume of 0.5193 cm3·g-1 on the basis of micropore volume around 0.1236 cm3·g-1, which was beneficial to the diffusion of reactant molecule; Raman spectra implied that there is a strong interaction between Ce and Ru. H2-TPR and O2-TPD showed that 5Ce0.5Ru/HZ-3 possessed the biggest consumption of hydrogen (0.486 mmol·g-1), surface adsorbed oxygen (0.683 mmol·g-1) and surface lattice oxygen (0.626 mmol·g-1), which was conducive to the adsorption and dissociation of reactant molecule; XPS showed 5Ce0.5Ru/HZ-3 had the biggest molar percentage of Ru4+ species (79.50%) and Ce3+ species (44.14%), which can induce the generation of much more oxygen vacancies. Overall, the introduction of Ce can result in the improvement of physical-chemical properties of 5Ce0.5Ru/HZ-3. Finally, the possible reaction route was given based on the in-situ DRIFTS and TD/GC-MS result.
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