ZHENG Qinzhong1,2, WU Xiaofeng1, CHEN Yunfa1,3
(1. State Key Laboratory of Multiphase Complex Systems; Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China; 2. School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China; 3. Center for Excellence in Regional Atmospheric Environment; Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China)
Abstract: Using chromium nitrate, terephthalic acid and hydrofluoric acid as raw materials, MIL-101(Cr) was prepared by hydrothermal method. The MnOx-Cr2O3 composite catalysts were subsequently prepared by high temperature pyrolysis by pre-impregnation with KMnO4 and reduction with H2O2.The catalytic activity of MnOx-Cr2O3 composite catalysts to benzene oxidation with different MnOx loading were characterized by BET、 XRD、 SEM、 TEM、 XPS. The results show that the addition of hydrofluoric acid plays a significant role in the pore structure of MIL-101(Cr)with high specific surface area. The MIL-101(Cr) prepared by adding 125 μL hydrofluoric acid has the best porosity, and its specific surface area reaches 3 447 m2/g after multiple activation with methanol. Specific surface area of high activity MnOx-Cr2O3 catalyst support is 89.30 m2/g, much higher than the commercial Cr2O3 support,andshows high catalytic activity for benzene oxidation (T90%=280 ℃).When the MnOx loading is 5%, the T90% of benzene being catalyzed is 266 ℃,but increasing the MnOx loading has little effect on the catalytic activity of the composite catalysts.The high catalytic activity of MnOx-Cr2O3 for benzene oxidation is attributed to the electron transfer between Mn and Cr, and the high surface lattice oxygen content. Good catalytic activity and non-toxic MnOx coating of MnOx-Cr2O3can inhibit the release of toxic Cr element.
Keywords: chromium oxide; manganese oxide; catalytic oxidation; volatile organic compounds
中图分类号:TB3
文献标志码:A
文章编号:1008-5548(2021)04-0054-09
DOI:10.13732/j.issn.1008-5548.2021.04.007
收稿日期: 2021-04-26, 修回日期:2021-05-08,在线出版时间:2021-06-01 09:40。
基金项目:国家自然科学基金项目,编号:51672273。
第一作者简介:郑钦中(1995—),男,硕士研究生,研究方向为纳米结构材料。E-mail:zheng-qz@qq.com。
通信作者简介:武晓峰(1978—),男,博士,研究员,博士生导师,研究方向为环境净化材料。E-mail:wxftsjc@ipe.ac.cn。