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室温下使用Mn-M双金属HZSM-5(M:Fe、Cu、Ru、Ag)催化剂对甲苯进行催化臭氧化。

Catalytic ozonation of toluene using Mn-M bimetallic HZSM-5 (M: Fe, Cu, Ru, Ag) catalysts at room temperature.

作者信息

Kim Jihee, Lee Jung Eun, Lee Hyung Won, Jeon Jong-Ki, Song JiHyeon, Jung Sang-Chul, Tsang Yiu Fai, Park Young-Kwon

机构信息

School of Environmental Engineering, University of Seoul, Seoul 02504, South Korea.

Department of Chemical Engineering, Kongju National University, Cheonan 31080, South Korea.

出版信息

J Hazard Mater. 2020 Oct 5;397:122577. doi: 10.1016/j.jhazmat.2020.122577. Epub 2020 May 5.

DOI:10.1016/j.jhazmat.2020.122577
PMID:32417604
Abstract

We investigated the catalytic efficiency of Mn-based bimetallic oxides in degrading toluene and ozone at room temperature. The room temperature-active bimetallic oxide catalysts were prepared by the addition of Fe, Cu, Ru, and Ag precursors to Mn/HZSM-5. We obtained H-temperature-programmed reduction (H-TPR) profiles, X-ray diffraction patterns, and X-ray photoelectron spectra to investigate the characteristics of the prepared catalysts. The catalytic efficiency of Mn-based bimetallic oxide catalysts in degrading toluene and ozone at room temperature was mostly improved by the addition of the secondary metals. The prepared bimetallic oxide catalysts, Cu-Mn/HZSM-5, Fe-Mn/HZSM-5, Ru-Mn/HZSM-5, and Ag-Mn/HZSM-5, enhanced efficiency for toluene removal compared to Mn/HZSM-5. The H-TPR profiles of the Mn-based bimetallic oxide catalysts showed stronger and broader adsorption-desorption bands at lower temperatures than the profile of Mn/HZSM-5. Additionally, the ratio of the surface defective oxygen over the lattice oxygen on the bimetallic oxide catalysts was higher than that of Mn-only catalysts; the ratio of Mn over Mn was higher for all bimetallic oxide catalysts, as well. Among the bimetallic oxide catalysts, Ru-Mn/HZSM-5 showed the highest efficiency for the removal of toluene to CO due to the synergetic effect of the oxidation state and reducible potential at room temperature.

摘要

我们研究了锰基双金属氧化物在室温下降解甲苯和臭氧的催化效率。通过向Mn/HZSM-5中添加铁、铜、钌和银前驱体制备了室温活性双金属氧化物催化剂。我们获得了氢程序升温还原(H-TPR)曲线、X射线衍射图谱和X射线光电子能谱,以研究制备的催化剂的特性。添加第二金属大多提高了锰基双金属氧化物催化剂在室温下降解甲苯和臭氧的催化效率。制备的双金属氧化物催化剂Cu-Mn/HZSM-5、Fe-Mn/HZSM-5、Ru-Mn/HZSM-5和Ag-Mn/HZSM-5与Mn/HZSM-5相比,提高了甲苯去除效率。锰基双金属氧化物催化剂的H-TPR曲线在较低温度下显示出比Mn/HZSM-5曲线更强、更宽的吸附-脱附带。此外,双金属氧化物催化剂上表面缺陷氧与晶格氧的比例高于仅含锰的催化剂;所有双金属氧化物催化剂中Mn/Mn的比例也更高。在双金属氧化物催化剂中,由于室温下氧化态和还原电位的协同作用,Ru-Mn/HZSM-5对甲苯氧化为CO的去除效率最高。

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