FeCoY催化剂的催化还原脱硫脱硝性能
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摘要
以CO为还原剂,FeCoY为活性组分,采用等体积浸渍法制备了一系列不同负载量、不同载体的催化剂FeCoY/AC,并在微型固定床反应器上探讨催化剂同时脱硫脱硝活性及抗氧化性。通过XRD、BET、H2-TPR对催化剂进行了表征。结果表明:经过硝酸预处理的催化剂能显著提高催化剂的性能;通过同时脱硫脱硝正交实验,得到活性组分Fe、Co、Y分别占载体质量10%、6%、3%的催化剂10Fe6Co3Y/AC为最优组合,脱硫脱硝转化率均能达100%,T90%(脱硫脱硝转化率同时达到90%时的温度)约为218℃。XRD结果表明:催化剂具有尖晶石结构。抗氧化性实验初步判断脱硫过程遵循Redox-COS协同作用机理,而脱硝仅遵循COS机理,体积分数为1%的O2对NO和SO2的活性位点表现出不同的毒害作用。
A series of catalysts with different loading amount and different supports were prepared by equal volume impregnation method using FeCoY as active component. Their simultaneous desulfurization and denitration activities and oxidation resistance were studied in an atmospheric pressure micro fixed bed reaction device using CO as reducing agent. The catalysts were characterized by XRD, BET and H2-TPR.The results show that pretreatment of activated carbon(AC) with nitric acid can improve the performance of the catalyst. The catalyst 10 Fe6Co3Y/AC(the active components Fe, Co and Y are 10%, 6% and 3% of the supports mass, respectively) is the best combination and the desulfurization and denitrification efficiencies can reach 100%. T90%(the temperature at which the desulfurization and denitrification efficiencies reach 90% simultaneously) is about 218 ℃. XRD results demonstrate that the catalyst has a spinel structure. From the results of oxidation resistance experiments, it is preliminarily judged that the desulfurization process follows the Redox-COS synergistic mechanism, while the denitration only follows the COS mechanism. Oxygen with a volume fraction of 1% exhibits different toxic effects on the active sites of NO and SO2.
A series of catalysts with different loading amount and different supports were prepared by equal volume impregnation method using FeCoY as active component. Their simultaneous desulfurization and denitration activities and oxidation resistance were studied in an atmospheric pressure micro fixed bed reaction device using CO as reducing agent. The catalysts were characterized by XRD, BET and H2-TPR.The results show that pretreatment of activated carbon(AC) with nitric acid can improve the performance of the catalyst. The catalyst 10 Fe6Co3Y/AC(the active components Fe, Co and Y are 10%, 6% and 3% of the supports mass, respectively) is the best combination and the desulfurization and denitrification efficiencies can reach 100%. T90%(the temperature at which the desulfurization and denitrification efficiencies reach 90% simultaneously) is about 218 ℃. XRD results demonstrate that the catalyst has a spinel structure. From the results of oxidation resistance experiments, it is preliminarily judged that the desulfurization process follows the Redox-COS synergistic mechanism, while the denitration only follows the COS mechanism. Oxygen with a volume fraction of 1% exhibits different toxic effects on the active sites of NO and SO2.
引文
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[16]Zhang Jinli(张锦丽).Experiments of desulfurization and denitrification andmechanism studies on desulfurization over modifiediron series oxides[D].Wuhan:Huazhong University of Science and Technology(华中科技大学),2014.
[17]Liu Zhaoqiong(刘赵穹),Ma Jun(马骏),Yang Xiyao(杨锡尧).SnO2-TiO2 solid solution catalyst for simultaneous reduction of SO2and NO by COⅢ.Catalyst active sites and reaction mechanism[J].Chinese Journal of Catalysis(催化学报),2004,25(8):624-632.
[18]Zhang Xiaoling(张晓玲).Study on simultaneous catalytic reduction of sulfur dioxide and nitric oxide on rare earth oxide[D].Wuhan:Huazhong University of Science and Technology(华中科技大学),2007.
[19]Song Yongji(宋永吉),Wang Ting(王婷),Zhao Yu(赵玉),et al.Desulfurization and denitrification performance of M-Y/AC catalysts[J].Journal of Fuel Chemistry and Technology(燃料化学学报),2016,44(9):1112-1118.
[20]Wang Xuehai(王学海),Fang Xiangchen(方向晨),Liu Zhongsheng(刘忠生).Simultaneous catalytic reduction of NO and SO2 with COover Fe/γ-Al2O3 catalysts[J].Industrial Catalysis(工业催化),2012,20(10):63-67.
[2]Li Hongqi(李鸿琦),Zhang Xiaolin(章小林),Li Xiaoding(李小定).Research development of flue gas desulfuration and denitrifictation integration technology[J].Power Technology and Environmental Protection(电力科技与环保),2014,30(3):14-15.
[3]Erdal Tan,Suatünal,Ali?an Do?an,et al.New“wet type”electron beam flue gas treatment pilot plant[J].Radiation Physics and Chemistry,2016,119:109-115.
[4]Xie G,Liu Z,Zhu Z,et al.Simultaneous removal of SO2,and NOx,from flue gas using a CuO/Al2O3,catalyst sorbent:I.Deactivation of SCR activity by SO2,at low temperatures[J].Journal of Catalysis,2004,224(1):36-41.
[5]Zhao Y,Han Y,Ma T,et al.Simultaneous desulfurization and denitrification from flue gas by Ferrate(Ⅵ)[J].Environmental Science&Technology,2011,45(9):4060.
[6]Hao R,Zhao Y,Yuan B,et al.Establishment of a novel advanced oxidation process for economical and effective removal of SO2 and NO[J].Journal of Hazardous Materials,2016,318:224-232.
[7]Guo S,Lv L,Jia Z,et al.Simultaneous removal of SO2 and NOx with ammonia combined with gas-phase oxidation of NO using ozone[J].Chemical Industry&Chemical Engineering Quarterly,2015,21(2):305-310.
[8]Shi Fenghua(史风华).Study on desulfurization and denitration with CO over rare earth oxide loaded on active carbon[D].Beijing:BeijingUniversity of Chemical Technology(北京化工大学),2013.
[9]Pantazis C C,Petrakis D E,Pomonis P J.Simultaneous and/or separate SO2/NO reduction by CO over high surface area Cu/Ce containing mesoporous silica[J].Applied Catalysis B:Environmental,2007,77(1/2):66-72.
[10]PengYaguang(彭亚光).Preparation of CexTi(1-x)O2 composite oxides and the research of desulfurization and denitrification performance[D].Central South University(中南大学),2014.
[11]Li Peng(李鹏),Ren Xiaoguang(任晓光),Liu Yining(刘怡宁).et al.Desulfuization and denitrifition properties of Cu O/γ-Al2O3catalysts[J].Industrial Catalysis(工业催化),2014,22(1):72-75.
[12]Wang Ting(王婷).A study on simultaneous desulfurization and denitrification by catalytic reduction method[D].Beijing:BeijingUniversity of Chemical Technology(北京化工大学),2016.
[13]Huang Wei(黄伟),Sun Shengkai(孙盛凯),Li Yujie(李玉杰),et al.Effects of nitric acid modification on the properties of activated carbon[J].Biomass Chemical Engineering(生物质化学工程),2006,40(6):17-21.
[14]Yang Chunyan(杨春雁),Zhang Xiwen(张喜文),Ling Fengxiang(凌凤香).Chemical adsorption instrument in the catalyst preparation process application[J].Liaoning Chemical Industry(辽宁化工),2004,33(11):645-648.
[15]Wen Bin(温斌).Simultaneous removal of the catalytic materials of NOx,SOx,and CO in FCC flue gas and their action principles[D].Beijing:Petroleum and Chemical Science Research Institute(石油化工科学研究院),2000.
[16]Zhang Jinli(张锦丽).Experiments of desulfurization and denitrification andmechanism studies on desulfurization over modifiediron series oxides[D].Wuhan:Huazhong University of Science and Technology(华中科技大学),2014.
[17]Liu Zhaoqiong(刘赵穹),Ma Jun(马骏),Yang Xiyao(杨锡尧).SnO2-TiO2 solid solution catalyst for simultaneous reduction of SO2and NO by COⅢ.Catalyst active sites and reaction mechanism[J].Chinese Journal of Catalysis(催化学报),2004,25(8):624-632.
[18]Zhang Xiaoling(张晓玲).Study on simultaneous catalytic reduction of sulfur dioxide and nitric oxide on rare earth oxide[D].Wuhan:Huazhong University of Science and Technology(华中科技大学),2007.
[19]Song Yongji(宋永吉),Wang Ting(王婷),Zhao Yu(赵玉),et al.Desulfurization and denitrification performance of M-Y/AC catalysts[J].Journal of Fuel Chemistry and Technology(燃料化学学报),2016,44(9):1112-1118.
[20]Wang Xuehai(王学海),Fang Xiangchen(方向晨),Liu Zhongsheng(刘忠生).Simultaneous catalytic reduction of NO and SO2 with COover Fe/γ-Al2O3 catalysts[J].Industrial Catalysis(工业催化),2012,20(10):63-67.
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