不同孔径HZSM-5协同低温等离子体催化降解甲苯性能研究  

Removal of toluene by non-thermal plasma combined with HZSM-5 zeolite:Effect of pore size

作　　者：陈扬达 王旎[1] 陈建东[1] 王冠男 吴军良[1,3,4] 付名利[1,3,4] 陈礼敏[1,3,4] 叶代启[1,3,4] CHEN Yangda WANG Ni CHEN Jiandong WANG Guannan WU Junliang FU Mingli CHEN Limin YE Daiqi(School of Environment and Energy, South China University of Technology, Guangzhou 510006 Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006 Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal, Guangzhou 510006 Guangzhou Hexin Instrument Co., Ltd,Guangzhou 510530)

机构地区：[1]华南理工大学环境与能源学院,广州510006 [2]广州禾信仪器股份有限公司,广州510530 [3]广东省大气环境与污染控制重点实验室,广州510006 [4]广东省环境风险防控与应急处置工程技术研究中心,广州510006

出　　处：《环境科学学报》2017年第2期503-511,共9页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.U1201231;51578245;51378218;51108187);国家高技术研究发展计划(No.2013AA065005);中央高校基本科研业务费专项基金;广州市科技计划项目(No.201510010164);2015年广东省公益研究与能力建设专项(No.2015A020215010);2014年广东省自然科学基金博士科研启动项目(No.2014A030310431)~~

摘　　要：研究了HZSM-5分子筛孔径对其在等离子体场内催化降解甲苯的影响.采用化学液相沉积法对HZSM-5分子筛进行改性,利用XRD、氮气吸附脱附等方法表征样品的骨架结构和表面性质,并用择形吸附实验对样品孔径进行表征.同时,评价了HZSM-5分子筛体系中降解甲苯的性能,研究了分子筛吸附甲苯性能及臭氧的产量,并采用飞行时间质谱(TOF-MS)和气相色谱-质谱联用仪(GC-MS)分析了反应产生的有机副产物.结果表明:液相沉积法成功调控了HZSM-5孔径,样品孔径随沉积剂用量增加而减小;同时,样品均具有相同的MFI骨架结构,比表面积和孔容相差不大.HZSM-5的孔径尺寸对甲苯去除率影响不大,但对碳平衡有影响,孔径越大,碳平衡越好.孔径较大的HZSM-5分子筛对甲苯具有更大的吸附速率和吸附容量,同时更多臭氧参与反应,生成·OH和O·,促进甲苯深度氧化,减少副产物,提高碳平衡.The HZSM-5 zeolites were prepared by chemical liquid-phase deposition method,and then characterized by X-ray diffraction（ XRD）,N2adsorption（ BET） and shape-selective adsorption test. The toluene removal efficiency over HZSM-5 zeolites was evaluated under a dielectric barrier discharge non-thermal plasma system. O3 productivity was measured by ozone analyzer,and organic products formed by oxidation were analyzed by TOFMS and GC-MS. The results showed that although the zeolites possessed different pore sizes,they had the same MFI structure,similar specific surface areaand pore volume. The pore size of HZSM-5 had little effects on the toluene removal efficiency; however,it could influence carbon balance,and larger pore size would result in better carbon balance. Toluene adsorption combined with O3 productivity,TOF-MS and GC-MS results indicated that HZSM-5 with larger pore size had a larger adsorption rate and adsorption capacity for toluene,while more O3 participated in the reaction,generating more ·OHand O·,which could promote the deep oxidation of toluene,reduce by-products and enhance carbon balance.

关 键 词：低温等离子体 HZSM-5 孔径 甲苯 

分 类 号：X701[环境科学与工程—环境工程]