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Understanding the correlation between calcination temperature and performance in low‐temperature methanation over Ni‐Zr/Al 2 O 3 catalysts
Author(s) -
Zhang Junfeng,
Zhang Meng,
Chen Shuyao,
Zhou Zeling,
Zheng Kaiwen,
Bai Yunxing,
Tan Yisheng,
Han Yizhuo
Publication year - 2020
Publication title -
the canadian journal of chemical engineering
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.404
H-Index - 67
eISSN - 1939-019X
pISSN - 0008-4034
DOI - 10.1002/cjce.23709
Subject(s) - methanation , calcination , catalysis , nial , non blocking i/o , spinel , materials science , nickel , x ray photoelectron spectroscopy , chemical engineering , inorganic chemistry , intermetallic , metallurgy , chemistry , organic chemistry , alloy , engineering
Abstract Low‐temperature methanation of CO in the continuous stirred tank reactor (CSTR) over Zr doped Ni/Al 2 O 3 catalyst calcined at different temperatures (673, 723, and 823 K) was investigated. XRD, TPR, XPS, ICP, SEM, and S ‐TPR techniques were employed to characterize the fresh and spent catalysts. Based on the characterization results, it was found that low‐temperature (673 K) calcination could effectively prohibit the formation of NiAl 2 O 4 spinel, thereby resulting in more reducible NiO particles, which were the essential precursor of methanation active sites over the catalyst surface. Thus, the highest CO conversion of 93.6% was achieved over the 25N3ZA‐673 catalyst. In addition, the deactivation rate of 25N3ZA‐673 was relatively slow in comparison to 25N3ZA‐823 due to the presence of more reducible NiO. The formed nickel carbonyl species (Ni[CO] x ), which quickly decomposed at a higher reaction temperature, was closely related to the catalyst deactivation. Therefore, 25N3ZA‐673 possessed much better stability at 593 K than that at 553 K.