Effects of Ni substitution on active oxygen species and electronic interactions over La0.8Ce0.2MnO3/mesoporous ZSM-5 for oxidizing C6H14

氧化剂 催化作用 化学 介孔材料 煅烧 X射线光电子能谱 氧气 己烷 无机化学 价(化学) 化学工程 有机化学 工程类
作者
Jian Li,Yao Shi,Xiaoheng Fu,Yun Shu,Jiayu Huang,Jinwei Zhu,Gang Tian,Jingnan Hu
出处
期刊:Molecular Catalysis [Elsevier]
卷期号:499: 111309-111309 被引量:8
标识
DOI:10.1016/j.mcat.2020.111309
摘要

Based on fly ash, mesoporous ZSM-5 (MZ) molecular sieves were prepared using a combination of hydrothermal treatment and fractional calcination. The La0.8Ce0.2Mn1-yNiyO3/MZ(y≤0.5) obtained using an impregnation load method was studied regarding the hexane oxidation, which was chosen as the probe molecule of volatile organic compounds (VOCs) at 120−390 °C. Additionally, the physicochemical characteristics of the catalysts were characterized by XRD, SEM, TEM, BET, XPS, NH3-TPD, H2-TPR and O2-TPD to investigate the electronic interactions over La0.8Ce0.2MnO3/MZ with Ni substitution and the active oxygen species, the main influence factors and the reaction mechanism for hexane oxidation. The results showed that there was a strong electronic interaction between LaMnO3 and MZ, and Ni substitution at Mn sites in La0.8Ce0.2MnO3 could promote the electronic transfer among the La, Ce, Ni, Mn and MZ, which could improve the low temperature reducibility, as well as facilitate the migration and distribution of the surface oxygen species. Additionally, La0.8Ce0.2Mn0.5Ni0.5O3/MZ demonstrated a higher catalytic activity for hexane oxidation due to its higher migration capacity of the outer lattice oxygen species (O2−), indicating that the outer lattice oxygen species as the active oxygen species were the main factor for hexane oxidation corresponding to the Mars-Van Krevelen (MvK) reaction mechanism. However, the specific surface area, the low temperature reducibility of high valence state cation ions (Mn4+ and/or Ni4+/Ni3+) and the surface acidity could be key but not main factors in hexane oxidation. Furthermore, La0.8Ce0.2Mn1-yNiyO3/MZ (y≤0.5) showed good catalytic stability, coke deposition resistance and H2O resistance. Based on the results of in situ DRIFTS and GC–MS, two reaction routes of hexane oxidation could be proposed over the La0.8Ce0.2Mn1-yNiyO3/MZ (y≤0.5) catalysts in air, therein, the decomposition of carbonate species could be one of the main rate- controlling steps at ≤ 320 °C.
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