Page 79 - 《精细化工》2022年第5期
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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。
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