The critical roles of hydrophobicity, surface Ru0 and active O2−/O22− sites on toluene combustion on Ru/ZSM-5 with varied Si/Al ratios

文献信息

发布日期 2022-05-16
DOI 10.1039/D2CP01476A
影响因子 3.676
作者

Jianjun Liu, Lanling Zeng, Xianglan Xu, Junwei Xu, Xiuzhong Fang, Yijun Bian, Xiang Wang


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摘要

By targeting more feasible catalysts for VOC combustion, 2%Ru/ZSM-5 catalysts were fabricated by supporting RuO2, a relatively cheaper noble metal, onto HZSM-5 supports with varied Si/Al ratios for toluene combustion. The valence state distribution of Ru and the Ru/RuO2-support interaction have been explored and elucidated. It has been revealed that the catalytic activity increases with the increase of the Si/Al ratio in the order 2%Ru/ZSM-5-18 < 2%Ru/ZSM-5-40 < 2%Ru/ZSM-5-72 < 2%Ru/ZSM-5-110 < 2%Ru/ZSM-5-255 < 2%Ru/SiO2-MFI. Interestingly, the hydrophobicity of the samples improves also with the increase in the Si/Al ratio, which impedes H2O adsorption effectively and its competition for the surface-active sites with the reactants. Both RuO2 and Ru0 are detected on all the catalysts, and the Ru0 amount/ratio increases significantly with increasing the Si/Al ratio, which promotes the adsorption/activation of both toluene and O2 molecules. Furthermore, the amount of surface-active O2− and O22− is evidently improved. Therefore, the mixed interaction of higher hydrophobicity, more surface Ru0 and active oxygen sites is the major reason for the enhancement in the activity of a Ru/ZSM-5 having a higher Si/Al ratio. It is concluded that the optimal catalyst can be designed by loading Ru/RuO2 onto an MFI framework structure support with the highest Si content.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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