Page 79 - 《精细化工》2022年第5期
P. 79
第 39 卷第 5 期 精 细 化 工 Vol.39, No.5
2022 年 5 月 FINE CHEMICALS May 2022
催化与分离提纯技术
Fe-Mn-CeO /AC@CNTs 催化剂低温
x
同时去除 NO 和氯苯
臧鹏超 1,2 ,吕学枚 1,2 ,刘 俊 1,2* ,王 影 1,2 ,张国杰 1,2* ,张永发 1,2
(1. 太原理工大学 化学化工学院,山西 太原 030024;2. 太原理工大学 省部共建煤基能源清洁高效利
用国家重点实验室,山西 太原 030024)
摘要:以活性炭@碳纳米管(AC@CNTs)为载体,通过浸渍法制备了 Mn-CeO x /AC@CNTs 催化剂,并考察了
铁物种的引入对 Mn-CeO x /AC@CNTs 催化剂同时去除 NO 和氯苯(CB)活性的影响。利用 SEM、XRD、Raman、
FTIR、XPS、H 2 -TPR 对催化剂的理化性质进行了表征。结果表明,Mn 物种进入 CeO 2 的晶格中形成 Mn-Ce 固
溶体促进氧空位的生成,而催化剂表面存在丰富的 C—H 基团和含氧基团有利于提高催化剂的低温催化活性。
与 Mn-CeO x (1∶7)/AC@CNTs〔n(Mn)∶n(Ce)=1∶7〕催化剂相比,Fe-Mn-CeO x (1∶7)/AC@CNTs 催化剂表面吸
附氧的含量和酸位点数量显著增加,使其具有良好的氧化还原性能和表面酸性。Fe-Mn-CeO x (1∶7)/AC@CNTs
催化剂在整个温度窗口表现出最高的催化活性,其中,在 225~300 ℃范围内,NO 转化率达到 90%以上,300 ℃
时,CB 转化率达 90%。此外,当 CB 存在时,300 ℃时,Fe-Mn-CeO x (1∶7)/AC@CNTs 催化剂的 NO 转化率仍
能达到 95%。
关键词:协同;氯苯;选择性催化还原;活性炭;碳纳米管;Mn-CeO x 氧化物催化剂;催化技术
中图分类号:X701;TQ426 文献标识码:A 文章编号:1003-5214 (2022) 05-0933-10
Fe-Mn-CeO x/AC@CNTs catalysts for simultaneous removal of
NO and chlorobenzene in low temperature
1,2
1,2
1,2
ZANG Pengchao , LYU Xuemei , LIU Jun 1,2* , WANG Ying ,
1,2
ZHANG Guojie 1,2* , ZHANG Yongfa
(1. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;
2. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024,
Shanxi, China)
Abstract: Carbon@carbon nanotubes (AC@CNTs) was used as support to prepare Mn-CeO x/AC@CNTs
catalyst by impregnation method. The effect of addition of Fe species on catalytic performance of
Mn-CeO x/AC@CNTs for the simultaneous nitrogen monoxide (NO) reduction and chlorobenzene (CB)
oxidation were investigated. The physical and chemical properties of catalyst were characterized by SEM,
XRD, Raman, FTIR, XPS and H 2-TPR. The results showed that Mn species entered the lattice of CeO 2 to
form Mn-Ce solid solution, which promoted the generation of oxygen vacancies. And abundant C—H
groups and oxygen-containing groups existing on the catalysts surface were beneficial to improve the
low-temperature catalytic activity. Compared with Mn-CeO x(1∶7)/AC@CNTs [n(Mn)∶n(Ce)=1∶7]
catalyst, Fe-Mn-CeO x(1∶7)/AC@CNTs catalyst exhibited better redox properties and surface acidity due
to its significantly increased oxygen adsorption content and acid site number. Fe-Mn-CeO x (1∶7)/AC@CNTs
catalyst showed the highest catalytic activity throughout the temperature window, with a NO conversion
over 90% at 225~300 ℃ and CB conversion was 90% at 300 ℃. In addition, the NO conversion over
收稿日期:2021-09-17; 定用日期:2021-12-23; DOI: 10.13550/j.jxhg.20210945
基金项目:博士后科学基金面上资助项目(2019M660061);山西省面上青年基金(201801D221349)
作者简介:臧鹏超(1996—),男,硕士生,E-mail:1584816294@qq.com。联系人:刘 俊(1987—),男,讲师,E-mail:xinzhou98010@
126.com;张国杰(1979—),男,教授,E-mail:zhgjdoc@126.com。