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)、H2程序升温还原(H2-TPR)、NH3程序升温脱附(NH3-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.
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 N2adsorption(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 ofSi/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 Ni O could promote the toluene oxidation,carbon dioxide selectivity and carbon balance,and decrease the formation of by-products in the process of plasma-catalysis.