Page 129 - 201809
P. 129
第 35 卷第 9 期 精 细 化 工 Vol.35, No.9
201 8 年 9 月 FINE CHEMICALS Sept. 2018
催化与分离提纯技术
自组装低负载量 Pd/γ-Al O 催化剂催化氧化甲苯
2
3
*
李 奔,周 贝,李思汉,严新焕
(浙江工业大学 绿色化学合成技术国家重点实验室培育基地,浙江 杭州 310014)
摘要:以 PdCl 2 和 Pd 2 (dba) 3 〔三(二亚苄基丙酮)二钯〕为前驱体,通过浸渍法、沉积沉淀法和自组装法分别
制备了负载量(质量分数,下同)为 0.03%的 Pd/γ-Al 2 O 3 -IM、Pd/γ-Al 2 O 3 -DP 和 Pd/γ-Al 2 O 3 -SA 催化剂用于催化
氧化甲苯。在甲苯体积分数为 0.1%、空速(SV)为 18000 mL/(g·h)条件下,Pd/γ-Al 2 O 3 -SA 催化剂上甲苯实现
98%转化率的温度(T 98 )为 220 ℃,比 Pd/γ-Al 2 O 3 -DP 和 Pd/γ-Al 2 O 3 -IM 分别降低了 40 和 75 ℃。通过 N 2 吸附-
脱附、XRD、TEM、XPS 和 H 2 -TPR 对催化剂进行了表征。结果表明:自组装法制备的 Pd/γ-Al 2 O 3 -SA 催化剂的
2
3
比表面积(345 m /g)和孔体积(0.52 cm /g)最大,Pd 纳米粒子(Pd NPs)平均粒径最小(5.0 nm),活性物种
主要以 PdO 的形式高度分散于载体 γ-Al 2 O 3 表面。此外,PdO 与载体 γ-Al 2 O 3 之间的强相互作用(SMSI)促进了其
催化氧化甲苯的活性。
关键词:自组装;Pd/γ-Al 2 O 3 ;催化氧化;甲苯;挥发性有机物;催化技术
中图分类号:O643;X13;X51 文献标识码:A 文章编号:1003-5214 (2018) 09-1555-07
A Self-assembled Pd/γ-Al 2O 3 Catalyst with Low Loading for
Catalytic Oxidation of Toluene
*
LI Ben, ZHOU Bei, LI Si-han, YAN Xin-huan
(State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology,
Hangzhou 310014, Zhejiang, China)
Abstract: Pd/γ-Al 2O 3-IM, Pd/γ-Al 2O 3-DP and Pd/γ-Al 2O 3-SA catalysts with 0.03% (mass fraction) Pd
loading for catalytic oxidation of toluene were respectively prepared by the impregnation,
deposition-precipition, and self-assembly methods using PdCl 2 and Pd 2(dba) 3 as precursors. The
temperature for conversion of 98% toluene (T 98) over Pd/γ-Al 2O 3-SA catalyst was 220 ℃ under the
conditions of toluene volume fraction at 0.1% and space velocity (SV) at 18000 mL/(g·h), which was 40
and 75 ℃ lower than those of Pd/γ-Al 2O 3- DP and Pd/γ-Al 2O 3-IM. The catalysts were characterized by N 2
adsorption-desorption, XRD, TEM, XPS, H 2-TPR. The results indicated that Pd/γ-Al 2O 3-SA catalyst
3
2
possessed the largest specific surface area (345 m /g) and pore volume (0.52 cm /g), the smallest average
diameter (5.0 nm) of Pd nanopaticles (NPs), and the main active PdO species were well-dispersed on the
surface of the γ-Al 2O 3 support. Besides, the strong metal-support interaction (SMSI) between PdO and
γ-Al 2O 3 promoted its performance in catalytic oxidation of toluene.
Key words: self-assembly; Pd/γ-Al 2O 3; catalytic oxidation; toluene; VOCs; catalysis technology
Foundation items: Plan Projects of Science & Technology in Zhejiang Province (2016C31104); the
National Key R&D Program of China (2017YFC0210900).
工业和运输过程中排放的挥发性有机化合物 气污染的主要成分之一 [1-2] 。催化氧化法是目前处理
(VOCs)是颗粒物(PM)和光化学烟雾的主要成 VOCs 最为经济有效的方式之一 [3-4] ,而研究与开发
因,因其通常具有恶臭味及毒性而被认为是造成空 相关催化剂是该技术的核心,并已成为环境催化研
收稿日期:2017-10-07; 定用日期:2018-02-01; DOI: 10.13550/j.jxhg.20170802
基金项目:浙江省科技计划项目(2016C31104);国家重点研发计划(2017YFC0210900)
作者简介:李 奔(1991—),男,硕士生。联系人:严新焕,教授,电话:0571-88320791,E-mail:xinhuanyan139@hotmail.com。