杨凤林1,
刘冰1
1.大连理工大学环境学院，工业生态与环境工程教育部重点实验室，大连 116024
Catalytic ozonation of NO by Mn-based catalysts using γ-Al2O3 as supporter at low temperature
TANG Yun1,,YANG Fenglin1,
LIU Bing1
1.Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
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摘要:利用等体积浸渍法制备γ-Al2O3负载Mn基催化剂，考察了掺杂元素种类，掺杂元素与Mn元素摩尔比以及煅烧温度对NO低温（100 ℃）催化氧化活性的影响，并对催化剂在有SO2或H2O的烟气中的稳定性进行了探究。结果表明，掺杂元素为Ce，Ce/Mn=0.4，煅烧温度为500 ℃条件下制备的催化剂NO催化活性最佳，在NO体积浓度为500×10-6，臭氧浓度为20.9 mg·L-1，n(O3)/n(NO)=0.2，反应温度为100 ℃，模拟烟气总流量为1.0 L·min-1，模拟烟气相对湿度为4%的条件下，NO的转化率最高可达70%。此外，还对催化剂在不同条件下的稳定性和活性恢复情况进行了探究。实验最终实现了在低O3浓度条件下达到较高NO转化率的目的，为烟气脱硝提供了一种具有应用潜力的新技术。
关键词: Mn基催化剂/
NO催化臭氧氧化/
低温/
稳定性/
活性恢复
Abstract:A series of Mn-based catalysts using γ-Al2O3 as supporter was prepared by incipient wetness impregnation. The effects of doping metal elements, the molar ratio of Ce/Mn and calcination temperature were investigated under low temperature (100 ℃) in this research. Moreover, the stablility of catalyst was tested in the simulated gas containing SO2 or H2O. The results suggested that MnOx-CeOx/γ-Al2O3 with mass ratio of 0.4 and calcination temperature of 500 ℃ got the highest activity at about 70% under the condition where initial concentration of NO was 500×10-6, inlet ozone concentration was 20.9 mg·L-1, the molar ratio of O3 and NO was 0.2, reaction temperature was 100 ℃，the total gas flow was 1.0 L·min-1 and relative humidity was 4%. Moreover, the stability under different situations and reactivation of catalyst was explored as well. Finally the experiment achieved a high conversion rate of NO under a low concentration of O3, which could be a new promising technology for denitrogenation from flue gas.
Key words:Mn-based catalyst/
catalytic ozonation of NO/
low temperature/
stability/
reactivation.
| [1] | ZHAO Y, WEN X Y, GUO T X, et al.Desulfurization and denitrogenation from flue gas using Fenton reagent[J].Fuel Processing Technology, 2014, 128: 54-60 10.1016/j.fuproc.2014.07.006 |
| [2] | KHAN N E, ADEWUYI Y G.Absorption and oxidation of nitric oxide (NO) by aqueous solution of sodium persulfate in a bubble column reactor[J].Industrial & Engineering Chemistry Research, 2010, 49: 8749-8760 10.1021/ie100607u |
| [3] | HUTSON N D, KRZYZYNSKA R, SRIVASTAVA R K.Simultaneous removal of SO2, NOx, and Hg from coal flue gas using a NaClO2-enhanced wet scrubber[J].Industrial & Engineering Chemistry Research, 2008, 47: 5825-5831 10.1021/ie800339p |
| [4] | ZHAO Y, GUO T X, CHEN Z Y, et al.Simultaneous removal of SO2 and NO using M/NaClO2 complex absorbent[J].Chemical Engineering Journal, 2010, 160: 42-47 10.1016/j.cej.2010.02.060 |
| [5] | FANG P, CEN C P, WANG X M, et al.Simultaneous removal of SO2, NO and HgO by wet scrubbing using urea+KMnO4 solution[J].Fuel Processing Technology, 2013, 106: 645-653 |
| [6] | ZHAO Y, HAO R L, ZHANG P, et al.Integrative process for simultaneous removal of SO2 and NO utilizing a vaporized H2O2/Na2S2O8[J].Energy & Fuels, 2014, 28: 6502-6510 10.1021/ef501686j |
| [7] | WANG Z H, LIN F W, JIANG S D, et al.Ceria substrate-oxide composites as catalyst for highly efficient catalytic oxidation of NO by O2[J].Fuel, 2016, 166: 352-360 10.1016/j.fuel.2015.11.012 |
| [8] | LIN F W, WANG Z H, MA Q, et al.Catalytic deep oxidation of NO by ozone over MnOx loaded spherical alumina catalyst[J].Applied Catalysis B: Environmental, 2016, 198: 100-111 10.1016/j.apcatb.2016.05.058 |
| [9] | LEE C L, LEE K T, ABDUL R M.Rice husk ash sorbent doped with copper for simultaneous removalof SO2 and NO: Optimization study[J].Journal of Hazardous Materials, 2010, 183: 738-745 10.1016/j.jhazmat.2010.07.088 |
| [10] | LEE C L, LEE K T, ABDUL R M.Effect of operating conditions towards simultaneous removal of SO2 and NO using copper modified rice husk ash: Role as sorbent and catalyst[J].Journal of Environmental Chemical Engineering, 2013, 11: 755-761 10.1016/j.jece.2013.07.017 |
| [11] | GAO X, JIANG Y, ZHONG Y, et al.The activity and characterization of CeO2-TiO2 catalysts prepared by the sol-gel method for selective catalytic reduction of NO with NH3[J].Journal of Hazardous Materials, 2010, 174: 734-739 10.1016/j.jhazmat.2009.09.112 |
| [12] | ZHANG Y L, ZHOU N B, PENG C, et al.Enhanced activity and stability of copper oxide/γ-alumina catalyst in catalytic wet-air oxidation: Critical roles of cerium incorporation[J].Applied Surface Science, 2018, 436: 981-988 10.1016/j.apsusc.2017.12.036 |
| [13] | 宋灿.不同晶形与形貌锰氧化物的合成及催化燃烧氯苯的研究[D].武汉：武汉工程大学，2012 |
| [14] | AGOLU R, PERALA V, DAMMA D, et al.Structural characteristics and catalytic performance of nanostructured Mn-doped CeO2 solid solutions towards oxidation of benzylamine by molecular O2[J].Materials Research Bulletin, 2017, 88: 136-147 10.1016/j.materresbull.2016.12.028 |
| [15] | LI X H, ZHANG S L, JIA Y, et al.Selective catalytic oxidation of NO with O2 over Ce-doped MnOx/TiO2 catalysts[J].Journal of Natural Gas Chemistry, 2012, 21: 17-24 10.1016/S1003-9953(11)60327-7 |
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γ-Al2O3负载Mn基催化剂低温催化臭氧氧化NO
唐云1,,杨凤林1,
刘冰1
1.大连理工大学环境学院，工业生态与环境工程教育部重点实验室，大连 116024
基金项目:
关键词: Mn基催化剂/
NO催化臭氧氧化/
低温/
稳定性/
活性恢复
摘要:利用等体积浸渍法制备γ-Al2O3负载Mn基催化剂，考察了掺杂元素种类，掺杂元素与Mn元素摩尔比以及煅烧温度对NO低温（100 ℃）催化氧化活性的影响，并对催化剂在有SO2或H2O的烟气中的稳定性进行了探究。结果表明，掺杂元素为Ce，Ce/Mn=0.4，煅烧温度为500 ℃条件下制备的催化剂NO催化活性最佳，在NO体积浓度为500×10-6，臭氧浓度为20.9 mg·L-1，n(O3)/n(NO)=0.2，反应温度为100 ℃，模拟烟气总流量为1.0 L·min-1，模拟烟气相对湿度为4%的条件下，NO的转化率最高可达70%。此外，还对催化剂在不同条件下的稳定性和活性恢复情况进行了探究。实验最终实现了在低O3浓度条件下达到较高NO转化率的目的，为烟气脱硝提供了一种具有应用潜力的新技术。
English Abstract
Catalytic ozonation of NO by Mn-based catalysts using γ-Al2O3 as supporter at low temperature
TANG Yun1,,YANG Fenglin1,
LIU Bing1
1.Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
Keywords: Mn-based catalyst/
catalytic ozonation of NO/
low temperature/
stability/
reactivation
Abstract:A series of Mn-based catalysts using γ-Al2O3 as supporter was prepared by incipient wetness impregnation. The effects of doping metal elements, the molar ratio of Ce/Mn and calcination temperature were investigated under low temperature (100 ℃) in this research. Moreover, the stablility of catalyst was tested in the simulated gas containing SO2 or H2O. The results suggested that MnOx-CeOx/γ-Al2O3 with mass ratio of 0.4 and calcination temperature of 500 ℃ got the highest activity at about 70% under the condition where initial concentration of NO was 500×10-6, inlet ozone concentration was 20.9 mg·L-1, the molar ratio of O3 and NO was 0.2, reaction temperature was 100 ℃，the total gas flow was 1.0 L·min-1 and relative humidity was 4%. Moreover, the stability under different situations and reactivation of catalyst was explored as well. Finally the experiment achieved a high conversion rate of NO under a low concentration of O3, which could be a new promising technology for denitrogenation from flue gas.
