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Influence of Calcination on Mesoporous Mn 1 Zr 0.5 O y Solid Solution in Oxidative Coupling Catalysis for Benzylideneaniline Formation
Author(s) -
Wu Shipeng,
Wei Kun,
Fang Wenhao
Publication year - 2021
Publication title -
chemistryselect
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.437
H-Index - 34
ISSN - 2365-6549
DOI - 10.1002/slct.202004509
Subject(s) - calcination , catalysis , physisorption , mesoporous material , chemistry , x ray photoelectron spectroscopy , inorganic chemistry , oxidative coupling of methane , aniline , yield (engineering) , nuclear chemistry , materials science , chemical engineering , organic chemistry , metallurgy , engineering
A mesoporous Mn 1 Zr 0.5 O y solid solution is prepared with a template‐free co‐precipitation method and is used as an efficient heterogeneous catalyst for oxidative coupling of benzyl alcohol and aniline in the absence of base under mild conditions. XRD, XPS, N 2 physisorption, H 2 ‐TPR, O 2 ‐TPD, NH 3 ‐TPD and CO 2 ‐TPD were used to study the influence of calcination temperature on the structure, redox properties, acidity‐basicity, as well as the catalytic behaviors of the Mn 1 Zr 0.5 O y catalyst. The results show that the optimal catalyst calcined at 400 °C displays the highest specific surface area (228 m 2 g −1 ), highest fraction of unsaturated Mn 3+ ions (45.4 %) and reactive O surf. species (52.5 %), and the highest acidity (1.06 mmol g −1 ) and basicity (0.48 mmol g −1 ). Thereby, an enhanced benzylideneaniline formation (5.50 mmol g cat −1 h −1 ) based on a 99 % yield is obtained at 80 °C under air atmosphere. This is one of the top results ever reported for all the Mn‐based catalysts. The structure‐activity relation is finally discussed.