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第 36 卷第 6 期 精 细 化 工 Vol.36, No.6
201 9 年 6 月 FINE CHEMICALS June 2019

催化与分离提纯技术
MO /Y 催化剂常温催化臭氧氧化甲苯的性能
x

黄金花 1,2,3 ，叶丽萍 1,2,3* ，罗 勇 1,2,3

（1. 上海化工研究院有限公司，上海 200062；2. 聚烯烃催化技术与高性能材料国家重点实验室，上海
200062；3. 上海市聚烯烃催化技术重点实验室，上海 200062）

摘要：以 Y 分子筛为载体，采用等体积浸渍法制备了 MO x /Y 催化剂，并用于常温催化臭氧氧化甲苯反应。采用
XRD、BET、H 2 -TPR、甲苯吸附对催化剂进行表征，以甲苯转化率维持 95%以上的时间（t 95 ）为指标对催化性
2
能进行评价。结果表明：10% MnO 2 /Y 催化剂〔m（MnO 2 ）/m（Y）=0.1〕具有较大的比表面积（538.6 m /g）
3
和孔容积（0.440 cm /g），较好的催化臭氧氧化甲苯活性（t 95 =210 min）；CuO 的加入提高了催化活性，5% MnO 2 -5%
CuO/Y 〔m(MnO 2 )/m(Y)=0.05 且 m(CuO)/m(Y)=0.05〕催化剂上 t 95 =240 min，CO x 选择性为 80.6%，CO 2 与 CO
摩尔比为 4.970。由表征结果可知，较大的比表面积和孔容积有利于甲苯吸附，CuO 与 MnO 2 之间的相互作用促
进了氧化还原性能的提高，进而有利于催化活性的提高。GC-MS 结果表明：反应副产物堵塞催化剂孔道，占据
催化剂表面活性位，导致催化剂失活。5% MnO 2 -5% CuO/Y 催化剂失活-再生 4 次后 t 95 可达 220 min。
关键词：常温；臭氧；甲苯；MnO 2 ；CuO；Y 分子筛；再生；催化技术
中图分类号：O643.3 文献标识码：A 文章编号：1003-5214 (2019) 06-1132-07

Catalytic performance of MO x/Y Catalyst for the Toluene
Oxidation with Ozone at Room Temperature

Huang Jin-hua 1,2,3 , Ye Li-ping 1,2,3* , Luo Yong 1,2,3
（1. Shanghai Research Institute of Chemical Industry Co., Ltd, Shanghai 200062, China; 2. State Key Laboratory of
Polyolefin and Catalysts, Shanghai 200062, China; 3. Shanghai Key Laboratory of Catalyst Technology for Polyolefin,
Shanghai 200062, China）

Abstract: A series of MO x/Y catalysts were prepared by incipient-wetness impregnation method with Y
zeolite as support for the toluene oxidation with ozone at room temperature. The catalysts were characterized
by XRD, BET, H 2-TPR and toluene adsorption techniques. The catalytic performance was evaluated by the
time (t 95) of toluene conversion rate above 95%. The results revealed that 10% MnO 2/Y〔m(MnO 2)/m(Y)
2
3
=0.1〕catalyst had a larger specific surface area of 538.6 m /g and pore volume of 0.440 cm /g, and
exhibited a better catalytic activity for toluene oxidation with ozone at room temperature. The addition of
CuO improved the catalytic activity of 5% MnO 2-5% CuO/Y〔m(MnO 2)/m(Y)=0.05 and m(CuO)/m(Y)=
0.05〕catalyst (t 95 of 240 min, CO x selectivity of 80.6%, and molar ratio of CO 2 to CO of 4.970). It was
found that larger surface area and pore volume promoted toluene adsorption, the interaction between CuO
and MnO 2 improved the reduction property of 10% MnO 2/Y catalyst. Thus, 5% MnO 2-5% CuO/Y catalyst
exhibited a high catalytic activity in the toluene oxidation with ozone at room temperature. GC-MS results
revealed that the by-products blocked the catalysts pores and occupied active sites on the surface of the
catalysts, resulting in the inactivation of the catalysts. The results of regeneration experiment indicated that
5% MnO 2-5% CuO/Y〔m(MnO 2)/m(Y)=0.05 and m(CuO)/m(Y)=0.05〕catalyst showed good catalytic
activity with t 95 of 220 min after regeneration for four times.
Key words: room temperature; ozone; toluene; MnO 2; CuO; Y zeolite; regeneration; catalysis technology

收稿日期：2018-09-19; 定用日期：2019-01-16; DOI: 10.13550/j.jxhg.20180698
作者简介：黄金花（1987—），女，工程师，硕士。联系人：叶丽萍（1981—），女，高工，博士，电话：021-52815377(1823)，E-mail：
ylp_by@126.com。