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Superior activity of Ce‐HZSM‐5 catalyst for catalytic oxidation of arsine at low oxygen
Author(s) -
Xie Yibing,
Wang Langlang,
Ning Ping,
Wang Xueqian,
Wang Qi,
Zhang Yingjie,
Wang Mengyu
Publication year - 2019
Publication title -
applied organometallic chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.53
H-Index - 71
eISSN - 1099-0739
pISSN - 0268-2605
DOI - 10.1002/aoc.4745
Subject(s) - catalysis , chemistry , x ray photoelectron spectroscopy , catalytic oxidation , oxygen , adsorption , inorganic chemistry , heterogeneous catalysis , nuclear chemistry , chemical engineering , organic chemistry , engineering
A series of Ce modified catalysts were prepared using equivalent‐volumetric ultrasonic impregnation method for AsH 3 removal. The performance of catalytic oxidation of AsH 3 under dynamic conditions was studied under different synthesis and reaction conditions. Through screening tests, the optimum catalyst was impregnated by 10 wt.% Ce (CH 3 COO) 3 precursor and subsequently calcinated at 550 °C. When the reaction temperature reached 170 °C, the Ce‐HZSM‐5 catalyst could maintain an oxidation efficiency of over 90% in 82 hrs. Furthermore, the chemical structure and properties of the catalyst and its catalytic oxidation mechanism with AsH 3 were analyzed using SEM‐EDS, BET, XRD, XPS, H 2 ‐TPR and FT‐IR. The results showed that Ce mainly existed on the catalyst surface in the forms of Ce 4+ and Ce 3+ . In the reaction process, the chemisorbed oxygen played a key role in the transformation between the two valence states. AsH 3 was firstly oxidized to elemental As with the participation of lattice oxygen. Then, the elemental As was partially blown into the rear part of the adsorption column along with the air flow and subsequently, de‐sublimed on the column wall. Herein, the elemental As remained on the surface of Ce‐HZSM‐5 catalyst, which would further oxidize to As 2 O 3 . For the recovery of As, Ce‐HZSM‐5 proved to be a promising catalyst in AsH 3 removal. Highlights The CeO x modified HZSM‐5 catalyst was used to catalytic oxidation of AsH 3 . The Ce‐HZSM‐5 catalyst could maintain over 90% oxidation efficiency in 82 hrs. AsH 3 was catalytic oxidized to elemental As and H 2 O on the catalyst surface and the As can be collected. The As adsorbed on the catalyst surface can be oxidized to As 2 O 3 but cannot be further oxidized to As 2 O 5 .