| 硅铝比和NiO对ZSM-5协同低温等离子体降解甲苯的影响 |
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| 引用本文： | 王旎,许伟城,肖海麟,徐晓鑫,王邦芬,吴军良,付名利,陈礼敏,叶代启.硅铝比和NiO对ZSM-5协同低温等离子体降解甲苯的影响[J].环境科学学报,2017,37(5):1884-1893. |
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| 作者姓名： | 王旎 许伟城 肖海麟 徐晓鑫 王邦芬 吴军良 付名利 陈礼敏 叶代启 |
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| 作者单位： | 华南理工大学环境与能源学院, 广州 510006,华南理工大学环境与能源学院, 广州 510006,华南理工大学环境与能源学院, 广州 510006,华南理工大学环境与能源学院, 广州 510006,华南理工大学环境与能源学院, 广州 510006,1. 华南理工大学环境与能源学院, 广州 510006;2. 广东省大气环境与污染控制重点实验室, 广州 510006;3. 广东省环境风险防控与应急处置工程技术研究中心, 广州 510006,1. 华南理工大学环境与能源学院, 广州 510006;2. 广东省大气环境与污染控制重点实验室, 广州 510006;3. 广东省环境风险防控与应急处置工程技术研究中心, 广州 510006,1. 华南理工大学环境与能源学院, 广州 510006;2. 广东省大气环境与污染控制重点实验室, 广州 510006;3. 广东省环境风险防控与应急处置工程技术研究中心, 广州 510006,1. 华南理工大学环境与能源学院, 广州 510006;2. 广东省大气环境与污染控制重点实验室, 广州 510006;3. 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 |
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| 基金项目： | 国家自然科学基金（No.U1201231，51378218，B5151050，5110818，51578245）；国家高技术研究发展计划（No.2013AA065005）；中央高校基本科研基金；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） |
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| 摘 要： | 研究了不同硅铝比的ZSM-5与Ni/ZSM-5分子筛协同低温等离子体技术对甲苯降解性能的影响.以Ni O(Nickel Oxide)为活性组分,采用浸渍法对ZSM-5分子筛进行改性,利用氮气吸附脱附(BET)、X射线衍射仪(XRD)、X射线光电子能谱分析(XPS)、H_2程序升温还原(H_2-TPR)、NH_3程序升温脱附(NH_3-TPD)、Toluene程序升温脱附(Toluene-TPD)等技术表征样品的物理化学性质.考察了硅铝比对ZSM-5与Ni/ZSM-5分子筛体系中甲苯的吸附性能,研究了不同放电电压下硅铝比对甲苯降解率、碳平衡及二氧化碳选择性的影响,并采用气相色谱-质谱联用仪(GC-MS)分析了催化剂表面的有机产物.结果表明:硅铝比不但影响分子筛本身的物理化学特性(比表面积、氧化还原性能、表面酸性、疏水性等),还会影响Ni的负载形态和方式,更高的硅铝比与Ni O的负载能促进甲苯深度氧化,减少副产物,提高碳平衡和二氧化碳选择性.
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| 关 键 词： | 低温等离子体 ZSM-5 硅铝比 甲苯 镍 |
| 收稿时间： | 2016/9/6 0:00:00 |
| 修稿时间： | 2017/2/9 0:00:00 |
Effects of Si/Al ratio and NiO on the interaction of non-thermal plasma and ZSM-5 catalysts |
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| WANG Ni,XU Weicheng,XIAO Hailin,XU Xiaoxin,WANG Bangfen,WU Junliang,FU Mingli,CHEN Limin and YE Daiqi.Effects of Si/Al ratio and NiO on the interaction of non-thermal plasma and ZSM-5 catalysts[J].Acta Scientiae Circumstantiae,2017,37(5):1884-1893. |
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| Authors: | WANG Ni XU Weicheng XIAO Hailin XU Xiaoxin WANG Bangfen WU Junliang FU Mingli CHEN Limin and YE Daiqi |
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| Institution: | School of Environment and Energy, South China University of Technology, Guangzhou 510006,School of Environment and Energy, South China University of Technology, Guangzhou 510006,School of Environment and Energy, South China University of Technology, Guangzhou 510006,School of Environment and Energy, South China University of Technology, Guangzhou 510006,School of Environment and Energy, South China University of Technology, Guangzhou 510006,1. School of Environment and Energy, South China University of Technology, Guangzhou 510006;2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006;3.Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006,1. School of Environment and Energy, South China University of Technology, Guangzhou 510006;2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006;3. Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006,1. School of Environment and Energy, South China University of Technology, Guangzhou 510006;2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006;3. Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006 and 1. School of Environment and Energy, South China University of Technology, Guangzhou 510006;2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006;3. Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006 |
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| Abstract: | Our study concentrated on the effect of different silica and alumina ratio (Si/Al) on ZSM-5 and Ni/ZSM-5 catalysts, and then analyzed their contribution to the toluene degradation under plasma activation. ZSM-5 doped with nickel oxide was synthesized by impregnation method, and then characterized by N2 adsorption (BET), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature program reduction (H2-TPR), NH3-temperature programmed desorption (NH3-TPD), Toluene-temperature programmed desorption (Toluene-TPD) and so on. The influences of Si/Al on ZSM-5 and Ni/ZSM-5 were investigated for the toluene adsorption capacity. Meanwhile, the toluene removal efficiency, carbon balance and carbon dioxide selectivity were evaluated under different discharge voltage and Si/Al in non-thermal plasma system. Moreover, organic products over the catalyst surface were analyzed by GC-MS. The results clearly demonstrated that the Si/Al is an essential parameter which could modify the physicochemical characteristics of zeolite itself and also influence the loading form of Ni. Higher Si/Al and the presence of NiO could promote the toluene oxidation, carbon dioxide selectivity and carbon balance, and decrease the formation of by-products in the process of plasma-catalysis. |
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| Keywords: | non-thermal plasma ZSM-5 ratio of silica and alumina toluene nickel |
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