团絮状双效催化聚苯硫醚滤料反应参数及机理
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摘要
以N-油酰基多肽表面活化聚苯硫醚滤料,以酸性KMn O_4在60～80℃操作温度下正向滴定,在氧化作用下实现活性组分氧化.实验研究了催化滤料的低温NO还原和Hg~0氧化性能,并通过SEM、EDX及TPD表征手段对催化滤料物化结构进行分析.分别考察了(0.9)Mn-Ce-Fe-Co-O_x/PPS反应体系温度、气相O_2浓度、初始NO浓度、氨氮比(NSR)、入口SO_2浓度的最佳反应参数.结果表明,有效组分Mn O_x、CeO_x、CoO_x、Fe_2O_3以团絮状均匀分散在纤维表面;在反应温度170℃、O_2≥5%、NO≤500×10~(-6)、氨氮比1.0、SO_2≤100 500×10~(-6)条件下,催化滤料对NO还原及Hg~0氧化效率基本达到80%左右;程序升温脱附实验Hg-TPD结果表明SO_2的Hg~0氧化促进作用机理于SO_3与Hg~0非均相反应优于SO_2硫酸化反应,而NO-TPD结果则表明NO与O_2在PPS表面相互作用类型以吸附态亚硝酸盐为主,吸附态NO_2次之.
The in-situ generation method was proposed to prepare the catalytic functional polyphenylene sulfide(PPS)filter material.PPS would be activated with C_(21)H_(40)NNa O_4S,and then treated in the metallic cations solution to adsorb Mn~(2+),Fe~(2+),Co~(2+),Ce~(3+)rapidly.After positive reaction with KMnO_4,reactive metal oxides were produced in the PPS materials.The(0.9)Mn-Ce-Fe-Co-O_x/PPS composite filter materials were characterized by SEM,EDX and TPD.Catalytic performance in the low-temperature catalytic conversion of NO and Hg~0 were then explored.The influences of reaction temperature,O_2,NO,ammonia-nitrogen ratio and SO_2 on the catalytic performance of catalytic PPS were investigated systematically.The results showed that MnO_x,CeO_x,CoO_x,Fe_2O_3 were uniformly distributed on the PPS filter material in a flocculent structure;The catalytic PPSmaterials performed a synergistically NO and Hg~0 removal efficiency of more than 80%in the conditions of T=170℃,O_2≥5%,NO≤500×10~(-6),NSR=1.0,SO_2≤100×10~(-6);The results of Hg-TPD desorption indicated that the mechanism of Hg~0 oxidation promotion of SO_2 was that the heterogeneous reaction between SO_3 and Hg~0 was faster than sulfation reaction of SO_2,and the NO-TPD results also showed that NO mainly acted in the form of nitrite on the surface of PPS,and followed by the form of adsorbed NO_2.
The in-situ generation method was proposed to prepare the catalytic functional polyphenylene sulfide(PPS)filter material.PPS would be activated with C_(21)H_(40)NNa O_4S,and then treated in the metallic cations solution to adsorb Mn~(2+),Fe~(2+),Co~(2+),Ce~(3+)rapidly.After positive reaction with KMnO_4,reactive metal oxides were produced in the PPS materials.The(0.9)Mn-Ce-Fe-Co-O_x/PPS composite filter materials were characterized by SEM,EDX and TPD.Catalytic performance in the low-temperature catalytic conversion of NO and Hg~0 were then explored.The influences of reaction temperature,O_2,NO,ammonia-nitrogen ratio and SO_2 on the catalytic performance of catalytic PPS were investigated systematically.The results showed that MnO_x,CeO_x,CoO_x,Fe_2O_3 were uniformly distributed on the PPS filter material in a flocculent structure;The catalytic PPSmaterials performed a synergistically NO and Hg~0 removal efficiency of more than 80%in the conditions of T=170℃,O_2≥5%,NO≤500×10~(-6),NSR=1.0,SO_2≤100×10~(-6);The results of Hg-TPD desorption indicated that the mechanism of Hg~0 oxidation promotion of SO_2 was that the heterogeneous reaction between SO_3 and Hg~0 was faster than sulfation reaction of SO_2,and the NO-TPD results also showed that NO mainly acted in the form of nitrite on the surface of PPS,and followed by the form of adsorbed NO_2.
引文
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