载体预处理对Fe-Mn/AC催化剂低温脱硝活性的影响
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摘要
以活性炭为载体,采用硝酸及热处理对载体进行预处理,用浸渍法制备Fe-Mn/AC催化剂,通过FTIR、SEM、N_2吸附-脱附、NH_3-TPD、H_2-TPR和XPS等进行表征,考察载体预处理对催化剂脱硝活性的影响。结果表明,载体预处理会影响载体的官能团、酸位、孔结构及比表面积等,进而影响活性组分的价态及分散性,活性组分的高价态和高分散性是其低温具有高活性的主要原因,载体经硝酸及300℃热处理的催化剂在140～250℃内活性提高近38%。
The activated carbon was used as carrier,and the carrier was pretreated by nitric acid and heat treatment.The Fe-Mn/AC catalyst was prepared by impregnation method and characterized by FTIR,SEM,N_2 adsorption-desorption,NH_3-TPD,H_2-TPR and XPS.The effect of carrier pretreatment on the denitrification activity of the catalyst was also investigated.The results show that the carrier pretreatment can affect the functional groups,acid sites,pore structure and specific surface area of the carrier,and futher affect the high valence and high dispersion of the active components.The high valence and high dispersion of active components are the main reasons for their high activity at low temperature.The activity of catalyst that the carrier was treated by nitric acid and 300 ℃ heat treatment increased by approximately 38% between 140 ℃ and 250 ℃.
The activated carbon was used as carrier,and the carrier was pretreated by nitric acid and heat treatment.The Fe-Mn/AC catalyst was prepared by impregnation method and characterized by FTIR,SEM,N_2 adsorption-desorption,NH_3-TPD,H_2-TPR and XPS.The effect of carrier pretreatment on the denitrification activity of the catalyst was also investigated.The results show that the carrier pretreatment can affect the functional groups,acid sites,pore structure and specific surface area of the carrier,and futher affect the high valence and high dispersion of the active components.The high valence and high dispersion of active components are the main reasons for their high activity at low temperature.The activity of catalyst that the carrier was treated by nitric acid and 300 ℃ heat treatment increased by approximately 38% between 140 ℃ and 250 ℃.
引文
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[2] Li C,Shen M,Wang J,et al.New insights into the promotional mechanism of ceria for activity and ammonium bisulfate resistance over V/WTi catalyst for selective catalytic reduction of NO with NH3[J].Applied Catalysis A:General,2018,560:153-164.
[3] Tang X,Li C,Yi H,et al.Facile and fast synthesis of novel Mn2CoO4@ rGO catalysts for the NH3-SCR of NOx at low temperature[J].Chemical Engineering Journal,2018,333:467-476.
[4] Liu Y,Zhao J,Lee J M.Conventional and new materials for selective catalytic reduction (SCR) of NOx[J].Chem Cat Chem,2018,10(7):1499-1511.
[5] Serrano-Lotina A,Bueno A C,Goberna-Selma C,et al.NO adsorption and influence of the control of temperature over catalytic test results for NO oxidation[J].Catalysis Today,2017,297:2-9.
[6] Chen J,Zhu B,Sun Y,et al.Investigation of low-temperature selective catalytic reduction of NOx with ammonia over Mn-modified Fe2O3/AC catalysts[J].Journal of the Brazilian Chemical Society,2018,29(1):79-87.
[7] Guo J X,Hu S,Liu X L,et al.Influence of Fe loadings on desulfurization performance of activated carbon treated by nitric acid[J].Environmental Technology,2017,38(3):266-276.
[8] 牟一蒙,梁红,李树华,等.焙烧温度对Mn/Al2O3-TiO2催化剂结构及氧化NO性能的影响[J].无机化学学报,2016,32(4):602-608.
[9] Pang F,Song F,Zhang Q,et al.Study on the influence of oxygen-containing groups on the performance of Ni/AC catalysts in methanol vapor-phase carbonylation[J].Chemical Engineering Journal,2016,293:129-138.
[10] Gao W,Zhang Z,Chen B,et al.Effects of calcination temperature on the structure and adsorption performance of Ce-Mn/AC materials[J].Wuhan University Journal of Natural Sciences,2017,22(5):435-442.
[11] 吴立军.改性柱状活性炭脱硫脱硝性能研究[D].马鞍山:安徽工业大学,2016.
[12] Jaramillo J,álvarez P M,Gómez-Serrano V.Preparation and ozone-surface modification of activated carbon.Thermal stability of oxygen surface groups[J].Applied Surface Science,2010,256(17):5232-5236.
[13] 姚瑞.活性炭低温催化氧化NO的研究[D].上海:华东理工大学,2015.
[14] 徐江海,潘红艳,王宁,等.N2高温热处理对活性炭孔道结构及表面化学性质的影响[J].炭素技术,2014,33(2):21-24.
[15] 王迪.制备过程和表面改性对煤质活性炭官能团影响规律研究[D].徐州:中国矿业大学,2014.
[16] Suprun W,Lutecki M,Haber T,et al.Acidic catalysts for the dehydration of glycerol:activity and deactivation[J].Journal of Molecular Catalysis A:Chemical,2009,309(1/2):71-78.
[17] Guo Q,Jing W,Hou Y,et al.On the nature of oxygen groups for NH3-SCR of NO over carbon at low temperatures[J].Chemical Engineering Journal,2015,270:41-49.
[18] Fang D,Xie J,Hu H,et al.Identification of MnOx species and Mn valence states in MnOx/TiO2 catalysts for low temperature SCR[J].Chemical Engineering Journal,2015,271:23-30.
[19] Wang T,Wan Z,Yang X,et al.Promotional effect of iron modification on the catalytic properties of Mn-Fe/ZSM-5 catalysts in the Fast SCR reaction[J].Fuel Processing Technology,2018,169:112-121.
[20] Thirupathi B,Smirniotis P G.Nickel-doped Mn/TiO2 as an efficient catalyst for the low-temperature SCR of NO with NH3:Catalytic evaluation and characterizations[J].Journal of Catalysis,2012,288:74-83.
[21] Liu Fudong,Asakura K,He Hong,et al.Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NOx with NH3[J].Applied Catalysis B:Environmental,2011,103(3):369-377.
[22] Yang Shijian,Wang Chizhong,Li Junhua,et al.Low temperature selective catalytic reduction of NO with NH3,over Mn-Fe spinel:Performance,mechanism and kinetic study[J].Applied Catalysis B:Environmental,2011,110(41):71-80.
[23] Yamashita T,Hayes P.Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials[J].Applied Surface Science,2008,254(8):2441-2449.
[24] Sutthiumporn K,Kawi S.Promotional effect of alkaline earth over Ni-La2O3 catalyst for CO2 reforming of CH4:role of surface oxygen species on H2 production and carbon suppression[J].International Journal of Hydrogen Energy,2011,36(22):14435-14446.