Cu改性Fe/Al-PILC催化剂的SCR-C_3H_6脱硝特性实验研究
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摘要
为提高Fe/Al-PILC催化剂的SCR脱硝的低温活性,采用Cu对Fe/Al-PILC催化剂进行改性。采用超声浸渍法合成系列x Cu-Fe/Al-PILC催化剂,通过XRD、N2吸附-脱附、H2-TPR、UV-vis、XPS、Py-FTIR等系列技术手段进行表征。在固定床微反应器上进行C3H6的选择性催化还原NO的实验。结果表明,经过铜改性后的x Cu-Fe/Al-PILC催化剂有效解决了Fe/Al-PILC催化剂低温SCR活性不足的问题,同时提高了中高温活性。催化剂在200-500℃能够实现80%以上脱硝效率,其中,0.13Cu-Fe/Al-PILC在250-500℃实现了90%以上NO转化率,并在250℃达到最高脱硝效率93%。XRD、N2吸附-脱附结果表明,经过铜改性的催化剂可以提供更多反应活性位,提高反应速率。H2-TPR结果表明,掺杂铜使催化剂获得低温还原能力,同时增强了中高温还原能力。UV-vis、XPS结果表明,铜掺杂不仅使铁获得更高氧化态,同时产生了更多低温活性物质孤立Fe~(3+)。Py-FTIR结果表明,催化剂表面同时存在Lewis酸和Br?nsted酸,Lewis酸是SCR反应活性中心。
In order to improve the lowtemperature activity of Fe/Al-PILC catalysts for SCR of NO,copper doping was used for the modification. x Cu-Fe/Al-PILC catalysts were prepared by ultrasonic impregnation technique and characterized by XRD,N_2 adsorption-desorption,H_2-TPR,UV-vis,XPS and Py-FTIR. The SCR of NO with C_3H_6 tests were carried out in a fixed bed reactor. The experimental results showed that the x Cu-Fe/Al-PILC catalysts can effectively solve the problem of insufficient SCR activity of Fe/Al-PILC catalysts at lowtemperature and as well as improve the activity at medium and high temperature. High NO reduction efficiency,80% and beyond could be achieved at a wide temperature range of 200-500 ℃ by the catalysts,among which0.13 Cu-Fe/Al-PILC exhibited 90% of the NO conversion at 250-500 ℃ and maximum NO reduction efficiency of 93% at 250 ℃. XRD and N_2 adsorption-desorption results proved that the catalysts modified by copper provided more active sites and increased the reaction rate. The results of H2-TPR indicated that the doping of copper improved the catalyst's redox ability at lower temperature,while enhanced the catalyst's redox ability at medium and high temperature. UV-vis and XPS study showed that the doping of copper not only increased the higher oxidation state of iron but also produced more isolated Fe~(3+) which is the low-temperature active species.Py-FTIR test illustrated that Lewis acid and Br?nsted acid existed simultaneously on the catalyst surface,and Lewis acid sites were the activity center of the SCR reaction.
In order to improve the lowtemperature activity of Fe/Al-PILC catalysts for SCR of NO,copper doping was used for the modification. x Cu-Fe/Al-PILC catalysts were prepared by ultrasonic impregnation technique and characterized by XRD,N_2 adsorption-desorption,H_2-TPR,UV-vis,XPS and Py-FTIR. The SCR of NO with C_3H_6 tests were carried out in a fixed bed reactor. The experimental results showed that the x Cu-Fe/Al-PILC catalysts can effectively solve the problem of insufficient SCR activity of Fe/Al-PILC catalysts at lowtemperature and as well as improve the activity at medium and high temperature. High NO reduction efficiency,80% and beyond could be achieved at a wide temperature range of 200-500 ℃ by the catalysts,among which0.13 Cu-Fe/Al-PILC exhibited 90% of the NO conversion at 250-500 ℃ and maximum NO reduction efficiency of 93% at 250 ℃. XRD and N_2 adsorption-desorption results proved that the catalysts modified by copper provided more active sites and increased the reaction rate. The results of H2-TPR indicated that the doping of copper improved the catalyst's redox ability at lower temperature,while enhanced the catalyst's redox ability at medium and high temperature. UV-vis and XPS study showed that the doping of copper not only increased the higher oxidation state of iron but also produced more isolated Fe~(3+) which is the low-temperature active species.Py-FTIR test illustrated that Lewis acid and Br?nsted acid existed simultaneously on the catalyst surface,and Lewis acid sites were the activity center of the SCR reaction.
引文
[1]IWAMOTO M,YAHIRO H,YU U Y.Selective reduction of NO by lower hydrocarbons in the presence of O2and SO2over copper ionexchanged zeolites[J].Cataly,1990,32(6):430-433.
[2]HELD W,KOENIG A,RICHTER T,PUPPE L.Catalytic NOxreduction in net oxidizing exhaust gas[J].SAE Trans,1990,99(4):209-216.
[3]GU H,CHUN K M,SONG S.The effects of hydrogen on the efficiency of NOxreduction via hydrocarbon-selective catalytic reduction(HC-SCR)at low temperature using various reductants[J].Int J Hydrogen Energy,2015,40(30):9602-9610.
[4]LI L D,GUAN N J.HC-SCR reaction pathways on ion exchanged ZSM-5 catalysts[J].Microporous Mesoporous Mater,2009,117(1/2):450-457.
[5]SCHURICHT F,RESCHETILOWSKI W.Simultaneous selective catalytic reduction(SCR)of NOxand N2O over Ag/ZSM-5-catalytic studies and mechanistic implications[J].Microporous Mesoporous Mater,2012,164:135-144.
[6]YAN S H,WANG X P,WANG W C,LIU Z Q,NIU J H.Selective catalytic reduction of NO by C2H2over Ce-Al2O3catalyst w ith ratedetermining step of NO oxidation[J].J Nat Gas Chem,2012,21(3):332-338.
[7]MORE P M,NGUYEN D L,GRANGER P,DUJARDIN C,DONGARE MK,UMBARKAR S B.Activation by pretreatment of Ag-Au/Al2O3bimetallic catalyst to improve low temperature HC-SCR of NOxfor lean burn engine exhaust[J].Appl Catal B:Environ,2015,174-175:145-156.
[8]周皞,苏亚欣,邓文义,钟方川.金属氧化物类催化剂上HC-SCR研究进展[J].环境科学与技术,2016,39(1):94-100.(ZHOU Hao,SU Ya-xin,DENG Wen-yi,ZHONG Fang-chuan.A review of HC-SCR over metal oxides-based catalysts[J].Environ Sci Technol,2016,39(1):94-100.)
[9]周皞,苏亚欣,邓文义,钟方川.负载金属分子筛类催化剂上HC-SCR研究进展[J].环境科学与技术,2015,38(10):64-73.(ZHOU Hao,SU Ya-xin,DENG Wen-yi,ZHONG Fang-chuan.A review of HC-SCR over metal-based zeolite catalysts[J].Environ Sci Technol,2015,38(10):64-73.)
[10]王琪莹,文焱炳,董新法,林维明.交联粘土合成及其在C3H6选择性催化还原NOx中的应用研究[J].高校化学工程学报,2006,4(20):598-603.(WANG Qi-ying,WEN Yan-bing,DONG Xin-fa,LIN Wei-ming.Application of pillared clays in selective catalytic reduction of NOxby C3H6[J].J Chem Eng Chin Univ,2006,4(20):598-603.)
[11]MENDIOROZ S,MART N-ROJO A B,RIVERA F,MART N J C,BAHAMONDE A,YATES M.Selective catalytic reduction of NOxby methane in excess oxygen over Rh based aluminium pillared clays[J].Appl Catal B:Environ,2006,64(3/4):161-170.
[12]YANG R T,THARAPPIWATTANANON N,LONG R Q.Ion-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J].Appl Catal B:Environ,1998,19(3/4):289-304.
[13]KONIN G A,IICHEV A N,MATYSHAK V A,KHOMENKO T I,KORCHAK V N,SADYKOV V A,DORONIN V P,BUNINA R V,ALIKINA G M,KUZNETSOVA T G,PAUKSHTIS E A,FENELONOV V B,ZAIKOVSKII V I,IVANOVA A S,BELOSHAPKIN S A,ROZOVSKII A Y,TRETYAKOV V F,ROSS J R H,BREEN J P.Cu,Co,Ag-containing pillared clays as catalysts for the selective reduction of NOxby hydrocarbons in an excess of oxygen[J].Top Catal,2001,16/17(1/4):193-197.
[14]ZHOU H,LI K K,ZHAO B T,DENG W Y,SU Y X,ZHONG F C.Surface properties and reactivity of Fe/Al2O3/cordierite catalysts for NO reduction by C2H6:Effects of calcination temperature[J].Chem Eng J,2017,326:737-744.
[15]ZHOU H,SU Y X,LIAO W Y,DENG W Y,ZHONG F C.Preparation,characterization,and properties of monolithic Fe/Al2O3/cordierite catalysts for NO reduction w ith C2H6[J].Appl Catal A:Gen,2015,505:402-409.
[16]苏亚欣,陆哲惺,周皞,窦逸峰,邓文义.丙烷在金属铁表面还原NO的实验研究[J].燃料化学学报,2014,42(12):1470-1477.(SU Ya-xin,LU Zhe-xing,ZHOU Hao,DOU Yi-feng,DENG Wen-yi.Experimental study on NO reduction by propane over iron[J].J Fuel Chem Technol,2014,42(12):1470-1476.)
[17]苏亚欣,苏阿龙,成豪.金属铁直接催化还原NO的实验研究[J].煤炭学报,2013,38(s1):206-210.(SU Ya-xin,SU A-long,CHENG Hao.Experimental study on direct catalytic reduction of NO by metallic iron[J].J China Coal Soc,2013,38(s1):206-210.)
[18]钱文燕,苏亚欣,杨溪,袁旻昊,邓文义,赵兵涛.Fe/Al-PILC催化C3H6选择性还原NO的实验研究[J].燃料化学学报,2017,45(12):1499-1507.(QIAN Wen-yan,SU Ya-xin,YANG Xi,YUAN Min-hao,DENG Wen-yi,ZHAO Bing-tao.Experimental study on selective catalytic reduction of NO w ith propene over iron based catalysts supported on aluminum pillared clays[J].J Fuel Chem Technol,2017,45(12):1499-1507.)
[19]YUAN MH,DENG W Y,DONG S L,LI Q C,ZHAO B T,SU Y X.Montmorillonite based porous clay heterostructures modified with Fe as catalysts for selective catalytic reduction of NO w ith propylene[J].Chem Eng J,2018,353:839-848.
[20]董士林,苏亚欣,刘欣,李前程,袁旻昊,周皞,邓文义.Fe/Ti-PILC用于C3H6选择性催化还原NO的研究[J].燃料化学学报,2018,46(10):1231-1239.(DONG Shi-lin,SU Ya-xin,LIU Xin,LI Qian-cheng,YUAN Min-hao,ZHOU Hao,DENG Wen-yi.Experimental study on selective catalytic reduction of NO by C3H6over Fe/Ti-PILC catalysts[J].J Fuel Chem Technol,2018,46(10):1231-1239.)
[21]SATO S,YU-U Y,YAHIRO H,MIZUNO N,IWAMOTO M.Cu-ZSM-5 zeolite as highly active catalyst for removal of nitrogen monoxide from emission of diesel engines[J].Appl Catal,1991,70(1):L1-L5.
[22]LI X Y,LU G,QU Z P,ZHANG D K,LIU S M.The role of titania pillar in copper-ion exchanged titania pillared clays for the selective catalytic reduction of NO by propylene[J].Appl Catal A:Gen,2011,398(1/2):82-87.
[23]LU G,LI X Y,QU Z P,ZHAO Q D,ZHAO L,CHEN G H.Copper-ion exchanged Ti-pillared clays for selective catalytic reduction of NOby propylene[J].Chem Eng J,2011,168(3):1128-1133.
[24]DORADO F,GARCA P B,DE LUCAS A,RAMOS MJ,ROMERO A.Hydrocarbon selective catalytic reduction of NO over Cu/Fepillared clays:Diffuse reflectance infrared spectroscopy studies[J].J Mol Catal A:Chem,2010,332(1/2):45-52.
[25]朱斌,费兆阳,陈献,汤吉海,崔咪芬,乔旭.Al-PILC负载铜铁复合氧化物选择性催化还原NO中的协同作用[J].燃料化学学报,2014,42(9):1102-1110.(ZHU Bin,FEI Zhao-yang,CHEN Xian,TANG Ji-hai,CUI Mi-fen,QIAO Xu.Synergetic effect of Cu-Fe composite oxides supported on Al-PILC for SCR of NO w ith NH3[J].J Fuel Chem Technol,2014,42(9):1102-1110.)
[26]VALVERDE J L,DE LUCAS A,SNCHEZ P,DORADO F,ROMERO A.Cation exchanged and impregnated Ti-pillared clays for selective catalytic reduction of NOxby propylene[J].Appl Catal B:Environ,2003,43(1):43-56.
[27]WANG Q Y,LIU Z L,WU J R.Effect of preparation methods on Ti-PILCs catalysts in selective catalytic reduction of NO by propylene[J].Adv Mater Res,2014,1033/1034:90-94.
[28]KIMB S,LEE S H,PARK Y T,HAMS W,CHAE H J,NAMI S.Selective catalytic reduction of NOxby propene over copper-exchanged pillared clays[J].Korean J Chem Eng,2001,18(5):704-710.
[29]文焱炳,董新法,林维明.Cu/Ce-Ti-PILC上丙烯选择催化还原NO的研究[J].广州大学学报(自然科学版),2008,7(1):53-57.(WEN Yan-bing,DONG Xin-fa,LIN Wei-min.Study on Cu/Ce-Ti-PILC for selective catalytic reduction of NO bypropylen[J].JGuangzhou Unv(Nat Sci Edi),2008,7(1):53-57.)
[30]QI G S,YANG R T.Selective catalytic oxidation(SCO)of ammonia to nitrogen over Fe/ZSM-5 catalysts[J].Appl Catal A:Gen,2005,287(1):25-33.
[31]KWAK J H,TONKYN R G,KIMD H,SZANYI J,PEDEN C H F.Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOxw ith NH3[J].J Catal,2010,275(2):187-190.
[32]XIA Y,ZHAN W C,GUO Y,GUO Y L,LU G Z.Fe-Beta zeolite for selective catalytic reduction of NOxw ith NH3:Influence of Fe content[J].Chin J Catal,2016,37(12):2069-2078.
[33]DELAHAY G,VALADE D,GUZMANVARGAS A,COQ B.Selective catalytic reduction of nitric oxide with ammonia on Fe-ZSM-5catalysts prepared by different methods[J].Appl Catal B:Environ,2005,55(2):149-155.
[34]LU R J,ZHANG X Y,MA C Y,WANG Z,WANG Y F,HAO Z P.Fe-Beta catalysts prepared by heating wet ion exchange and their catalytic performances on N2O catalytic decomposition and reduction[J].Asia-Pac J Chem Eng,2014,9(2):159-166.
[35]SCHWIDDER M,KUMAR MS,KLEMENTIEV K,POHL MM,BRCKNER A,GRNERT W.Selective reduction of NO with Fe-ZSM-5 catalysts of low Fe content.Relations betw een active site structure and catalytic performance[J].J Catal,2005,231(2):314-330.
[36]OLIVEIRA L C A,RIOS R V R A,FABRIS J D,SAPAG K,GARG V K,LAGO R M.Clay-iron oxide magnetic composites for the adsorption of contaminants in w ater[J].Appl Clay Sci,2003,22(4):169-177.
[37]DORADO F,DE LUCAS A,GARCA P B,ROMERO A,VALVERDE J L.Copper ion-exchanged and impregnated Fe-pillared clays Study of the influence of the synthesis conditions on the activity for the selective catalytic reduction of NO w ith C3H6[J].Appl Catal A:Gen,2006,305(2):189-196.
[38]YANG R T,THARAPPIWATTANANON N,LONG R Q.Ion-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J].Appl Catal B:Environ,1998,19(3/4):289-304.
[39]JIN Y M,DATYE A K.Phase transformations in iron Fischer-Tropsch catalysts during temperature programmed reduction[J].J Catal,2000,196(1):8-17.
[40]SUN MM,CAO Y,LAN L,ZOU S,FANG Z T,CHEN Y Q.Selective catalytic oxidation of ammonia to nitrogen over iron and copper bimetallic catalysts[J].Acta Phys-Chim Sin,2014,30(12):2300-2306.
[41]KUMAR MS,SCHWIDDER M,GRNERT W,BRCKNER A.On the nature of different iron sites and their catalytic role in Fe-ZSM-5DeNOxcatalysts:New insights by a combined EPR and UV/VIS spectroscopic approach[J].J Catal,2004,227(2):384-397.
[42]LU L,LI L,WANG X,LI G.Understanding of the finite size effects on lattice vibrations and electronic transitions of nano alpha-Fe2O3.[J].J Phys Chem B,2005,109(36):17151-17156.
[43]TIPPINS H H.Charge-transfer spectra of transition-metal ions in corundum[J].Phys Rev B,1970,1(1):126-135.
[44]GIORDANINO F,VENNESTROMP N R LUNDEGAARD L F,STAPPEN F N,MOSSIN S,BEATO P,BORDIGA S,LAMBERTI C.Characterization of Cu-exchanged SSZ-13:A comparative FT-IR,UV-Vis and EPR study w ith Cu-ZSM-5 and Cu-beta w ith similar Si/Al and Cu/Al ratios[J].Dalton Trans,2013,42(35):12741-12761.
[45]ISMAGILOV Z R,YASHNIK S A,ANUFRIENKO V F,LARINA T V,VASENIN N T,BULGAKOV N N,VOSELET S V,TSYKOZAL T.Linear nanoscale clusters of CuO in Cu-ZSM-5 catalysts[J].Appl Surf Sci,2004,226(1/3):88-93.
[46]KIMMH,NAMI-S,KIMY G.Characteristics of mordenite-type zeolite catalysts deactivated by SO2for the reduction of NO w ith hydrocarbons[J].J Catal,1998,179(2):350-360.
[47]CHADWICK D,HASHEMI T.Adsorbed corrosion inhibitors studied by electron spectroscopy:Benzotriazole on copper and copper alloys[J].Corros Sci,1978,18(1):39-51.
[48]GONG J L,YUE H R,ZHAO Y J,ZHAO S,ZHAO L,LV J,WANG S P,MA X B.Synthesis of ethanol via syngas on Cu/SiO2catalysts w ith balanced Cu0-Cu+sites[J].J Am Chem Soc,2012,134(34):13922-13925.
[49]GUO H J,ZHANG H R,PENG F,YANG H J,XIONG L,WANG C,HUANG C,CHEN X D,MA L L.Effects of Cu/Fe ratio on structure and performance of attapulgite supported CuFeCo-based catalyst for mixed alcohols synthesis from syngas[J].Appl Catal A:Gen,2015,503(25):51-61.
[50]LI F,ZHANG L H,EVANS D G,DUAN X.Structure and surface chemistry of manganese-doped copper-based mixed metal oxides derived from layered double hydroxides[J].Colloids Surf A,2004,244(1/3):169-177.
[51]DATKA J,TUREK A M,JEHNG J M,WACHS I E.Acidic properties of supported niobium oxide catalysts:An infrared spectroscopy investigation[J].J Catal,1992,135(1):186-199.
[52]BARZETTI T,SELLI E,MOSCOTTI D,FORNI L.Pyridine and ammonia as probes for FT-IR analysis of solid acid catalysts[J].J Chem Soc Faraday Trans,1996,92(8):1401-1407.
[53]SULTANA A,HANEDA M,FUJITANI T,HAMADA H.Influence of Al2O3support on the activity of Ag/Al2O3catalysts for SCR of NOw ith decane[J].Catal Lett,2007,114(1/2):96-102.
[54]CHMIELARZ L,PIWOWARSKA Z,KU'S TROWSKI P,WEGRZYN A,GIL B,KOWALCZYK A,DUDEK B,DZIEMBAJ R,MICHALIKET M.Comparison study of titania pillared interlayered clays and porous clay heterostructures modified w ith copper and iron as catalysts of the DeNOxprocess[J].Appl Clay Sci,2011,53(2):164-173.
[55]LONG R Q,YANG R T.Selective catalytic reduction of nitrogen oxides by ammonia over Fe3+-Exchanged TiO2-pillared clay catalysts[J].JCatal,1999,186(2):254-268.
[56]EMEIS C A.Determination of integrated molar extinction coefficients for infrared absorption bands of pyridine absorbed on solid acid catalysts[J].J Catal,1993,141(2):347-354.
[57]LI J H,ZHU Y Q,KE R,HAO J M.Improvement of catalytic activity and sulfur-resistance of Ag/TiO2-Al2O3for NO reduction w ith propene under lean burn conditions[J].Appl Catal B:Environ,2008,80(3/4):202-213.
[58]DATKA J,GIL B,KUBACKA A.Heterogeneity of OH groups in H-mordenites:Effect of dehydroxylation[J].Zeolites,1996,17(5/6):428-433.
[2]HELD W,KOENIG A,RICHTER T,PUPPE L.Catalytic NOxreduction in net oxidizing exhaust gas[J].SAE Trans,1990,99(4):209-216.
[3]GU H,CHUN K M,SONG S.The effects of hydrogen on the efficiency of NOxreduction via hydrocarbon-selective catalytic reduction(HC-SCR)at low temperature using various reductants[J].Int J Hydrogen Energy,2015,40(30):9602-9610.
[4]LI L D,GUAN N J.HC-SCR reaction pathways on ion exchanged ZSM-5 catalysts[J].Microporous Mesoporous Mater,2009,117(1/2):450-457.
[5]SCHURICHT F,RESCHETILOWSKI W.Simultaneous selective catalytic reduction(SCR)of NOxand N2O over Ag/ZSM-5-catalytic studies and mechanistic implications[J].Microporous Mesoporous Mater,2012,164:135-144.
[6]YAN S H,WANG X P,WANG W C,LIU Z Q,NIU J H.Selective catalytic reduction of NO by C2H2over Ce-Al2O3catalyst w ith ratedetermining step of NO oxidation[J].J Nat Gas Chem,2012,21(3):332-338.
[7]MORE P M,NGUYEN D L,GRANGER P,DUJARDIN C,DONGARE MK,UMBARKAR S B.Activation by pretreatment of Ag-Au/Al2O3bimetallic catalyst to improve low temperature HC-SCR of NOxfor lean burn engine exhaust[J].Appl Catal B:Environ,2015,174-175:145-156.
[8]周皞,苏亚欣,邓文义,钟方川.金属氧化物类催化剂上HC-SCR研究进展[J].环境科学与技术,2016,39(1):94-100.(ZHOU Hao,SU Ya-xin,DENG Wen-yi,ZHONG Fang-chuan.A review of HC-SCR over metal oxides-based catalysts[J].Environ Sci Technol,2016,39(1):94-100.)
[9]周皞,苏亚欣,邓文义,钟方川.负载金属分子筛类催化剂上HC-SCR研究进展[J].环境科学与技术,2015,38(10):64-73.(ZHOU Hao,SU Ya-xin,DENG Wen-yi,ZHONG Fang-chuan.A review of HC-SCR over metal-based zeolite catalysts[J].Environ Sci Technol,2015,38(10):64-73.)
[10]王琪莹,文焱炳,董新法,林维明.交联粘土合成及其在C3H6选择性催化还原NOx中的应用研究[J].高校化学工程学报,2006,4(20):598-603.(WANG Qi-ying,WEN Yan-bing,DONG Xin-fa,LIN Wei-ming.Application of pillared clays in selective catalytic reduction of NOxby C3H6[J].J Chem Eng Chin Univ,2006,4(20):598-603.)
[11]MENDIOROZ S,MART N-ROJO A B,RIVERA F,MART N J C,BAHAMONDE A,YATES M.Selective catalytic reduction of NOxby methane in excess oxygen over Rh based aluminium pillared clays[J].Appl Catal B:Environ,2006,64(3/4):161-170.
[12]YANG R T,THARAPPIWATTANANON N,LONG R Q.Ion-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J].Appl Catal B:Environ,1998,19(3/4):289-304.
[13]KONIN G A,IICHEV A N,MATYSHAK V A,KHOMENKO T I,KORCHAK V N,SADYKOV V A,DORONIN V P,BUNINA R V,ALIKINA G M,KUZNETSOVA T G,PAUKSHTIS E A,FENELONOV V B,ZAIKOVSKII V I,IVANOVA A S,BELOSHAPKIN S A,ROZOVSKII A Y,TRETYAKOV V F,ROSS J R H,BREEN J P.Cu,Co,Ag-containing pillared clays as catalysts for the selective reduction of NOxby hydrocarbons in an excess of oxygen[J].Top Catal,2001,16/17(1/4):193-197.
[14]ZHOU H,LI K K,ZHAO B T,DENG W Y,SU Y X,ZHONG F C.Surface properties and reactivity of Fe/Al2O3/cordierite catalysts for NO reduction by C2H6:Effects of calcination temperature[J].Chem Eng J,2017,326:737-744.
[15]ZHOU H,SU Y X,LIAO W Y,DENG W Y,ZHONG F C.Preparation,characterization,and properties of monolithic Fe/Al2O3/cordierite catalysts for NO reduction w ith C2H6[J].Appl Catal A:Gen,2015,505:402-409.
[16]苏亚欣,陆哲惺,周皞,窦逸峰,邓文义.丙烷在金属铁表面还原NO的实验研究[J].燃料化学学报,2014,42(12):1470-1477.(SU Ya-xin,LU Zhe-xing,ZHOU Hao,DOU Yi-feng,DENG Wen-yi.Experimental study on NO reduction by propane over iron[J].J Fuel Chem Technol,2014,42(12):1470-1476.)
[17]苏亚欣,苏阿龙,成豪.金属铁直接催化还原NO的实验研究[J].煤炭学报,2013,38(s1):206-210.(SU Ya-xin,SU A-long,CHENG Hao.Experimental study on direct catalytic reduction of NO by metallic iron[J].J China Coal Soc,2013,38(s1):206-210.)
[18]钱文燕,苏亚欣,杨溪,袁旻昊,邓文义,赵兵涛.Fe/Al-PILC催化C3H6选择性还原NO的实验研究[J].燃料化学学报,2017,45(12):1499-1507.(QIAN Wen-yan,SU Ya-xin,YANG Xi,YUAN Min-hao,DENG Wen-yi,ZHAO Bing-tao.Experimental study on selective catalytic reduction of NO w ith propene over iron based catalysts supported on aluminum pillared clays[J].J Fuel Chem Technol,2017,45(12):1499-1507.)
[19]YUAN MH,DENG W Y,DONG S L,LI Q C,ZHAO B T,SU Y X.Montmorillonite based porous clay heterostructures modified with Fe as catalysts for selective catalytic reduction of NO w ith propylene[J].Chem Eng J,2018,353:839-848.
[20]董士林,苏亚欣,刘欣,李前程,袁旻昊,周皞,邓文义.Fe/Ti-PILC用于C3H6选择性催化还原NO的研究[J].燃料化学学报,2018,46(10):1231-1239.(DONG Shi-lin,SU Ya-xin,LIU Xin,LI Qian-cheng,YUAN Min-hao,ZHOU Hao,DENG Wen-yi.Experimental study on selective catalytic reduction of NO by C3H6over Fe/Ti-PILC catalysts[J].J Fuel Chem Technol,2018,46(10):1231-1239.)
[21]SATO S,YU-U Y,YAHIRO H,MIZUNO N,IWAMOTO M.Cu-ZSM-5 zeolite as highly active catalyst for removal of nitrogen monoxide from emission of diesel engines[J].Appl Catal,1991,70(1):L1-L5.
[22]LI X Y,LU G,QU Z P,ZHANG D K,LIU S M.The role of titania pillar in copper-ion exchanged titania pillared clays for the selective catalytic reduction of NO by propylene[J].Appl Catal A:Gen,2011,398(1/2):82-87.
[23]LU G,LI X Y,QU Z P,ZHAO Q D,ZHAO L,CHEN G H.Copper-ion exchanged Ti-pillared clays for selective catalytic reduction of NOby propylene[J].Chem Eng J,2011,168(3):1128-1133.
[24]DORADO F,GARCA P B,DE LUCAS A,RAMOS MJ,ROMERO A.Hydrocarbon selective catalytic reduction of NO over Cu/Fepillared clays:Diffuse reflectance infrared spectroscopy studies[J].J Mol Catal A:Chem,2010,332(1/2):45-52.
[25]朱斌,费兆阳,陈献,汤吉海,崔咪芬,乔旭.Al-PILC负载铜铁复合氧化物选择性催化还原NO中的协同作用[J].燃料化学学报,2014,42(9):1102-1110.(ZHU Bin,FEI Zhao-yang,CHEN Xian,TANG Ji-hai,CUI Mi-fen,QIAO Xu.Synergetic effect of Cu-Fe composite oxides supported on Al-PILC for SCR of NO w ith NH3[J].J Fuel Chem Technol,2014,42(9):1102-1110.)
[26]VALVERDE J L,DE LUCAS A,SNCHEZ P,DORADO F,ROMERO A.Cation exchanged and impregnated Ti-pillared clays for selective catalytic reduction of NOxby propylene[J].Appl Catal B:Environ,2003,43(1):43-56.
[27]WANG Q Y,LIU Z L,WU J R.Effect of preparation methods on Ti-PILCs catalysts in selective catalytic reduction of NO by propylene[J].Adv Mater Res,2014,1033/1034:90-94.
[28]KIMB S,LEE S H,PARK Y T,HAMS W,CHAE H J,NAMI S.Selective catalytic reduction of NOxby propene over copper-exchanged pillared clays[J].Korean J Chem Eng,2001,18(5):704-710.
[29]文焱炳,董新法,林维明.Cu/Ce-Ti-PILC上丙烯选择催化还原NO的研究[J].广州大学学报(自然科学版),2008,7(1):53-57.(WEN Yan-bing,DONG Xin-fa,LIN Wei-min.Study on Cu/Ce-Ti-PILC for selective catalytic reduction of NO bypropylen[J].JGuangzhou Unv(Nat Sci Edi),2008,7(1):53-57.)
[30]QI G S,YANG R T.Selective catalytic oxidation(SCO)of ammonia to nitrogen over Fe/ZSM-5 catalysts[J].Appl Catal A:Gen,2005,287(1):25-33.
[31]KWAK J H,TONKYN R G,KIMD H,SZANYI J,PEDEN C H F.Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOxw ith NH3[J].J Catal,2010,275(2):187-190.
[32]XIA Y,ZHAN W C,GUO Y,GUO Y L,LU G Z.Fe-Beta zeolite for selective catalytic reduction of NOxw ith NH3:Influence of Fe content[J].Chin J Catal,2016,37(12):2069-2078.
[33]DELAHAY G,VALADE D,GUZMANVARGAS A,COQ B.Selective catalytic reduction of nitric oxide with ammonia on Fe-ZSM-5catalysts prepared by different methods[J].Appl Catal B:Environ,2005,55(2):149-155.
[34]LU R J,ZHANG X Y,MA C Y,WANG Z,WANG Y F,HAO Z P.Fe-Beta catalysts prepared by heating wet ion exchange and their catalytic performances on N2O catalytic decomposition and reduction[J].Asia-Pac J Chem Eng,2014,9(2):159-166.
[35]SCHWIDDER M,KUMAR MS,KLEMENTIEV K,POHL MM,BRCKNER A,GRNERT W.Selective reduction of NO with Fe-ZSM-5 catalysts of low Fe content.Relations betw een active site structure and catalytic performance[J].J Catal,2005,231(2):314-330.
[36]OLIVEIRA L C A,RIOS R V R A,FABRIS J D,SAPAG K,GARG V K,LAGO R M.Clay-iron oxide magnetic composites for the adsorption of contaminants in w ater[J].Appl Clay Sci,2003,22(4):169-177.
[37]DORADO F,DE LUCAS A,GARCA P B,ROMERO A,VALVERDE J L.Copper ion-exchanged and impregnated Fe-pillared clays Study of the influence of the synthesis conditions on the activity for the selective catalytic reduction of NO w ith C3H6[J].Appl Catal A:Gen,2006,305(2):189-196.
[38]YANG R T,THARAPPIWATTANANON N,LONG R Q.Ion-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J].Appl Catal B:Environ,1998,19(3/4):289-304.
[39]JIN Y M,DATYE A K.Phase transformations in iron Fischer-Tropsch catalysts during temperature programmed reduction[J].J Catal,2000,196(1):8-17.
[40]SUN MM,CAO Y,LAN L,ZOU S,FANG Z T,CHEN Y Q.Selective catalytic oxidation of ammonia to nitrogen over iron and copper bimetallic catalysts[J].Acta Phys-Chim Sin,2014,30(12):2300-2306.
[41]KUMAR MS,SCHWIDDER M,GRNERT W,BRCKNER A.On the nature of different iron sites and their catalytic role in Fe-ZSM-5DeNOxcatalysts:New insights by a combined EPR and UV/VIS spectroscopic approach[J].J Catal,2004,227(2):384-397.
[42]LU L,LI L,WANG X,LI G.Understanding of the finite size effects on lattice vibrations and electronic transitions of nano alpha-Fe2O3.[J].J Phys Chem B,2005,109(36):17151-17156.
[43]TIPPINS H H.Charge-transfer spectra of transition-metal ions in corundum[J].Phys Rev B,1970,1(1):126-135.
[44]GIORDANINO F,VENNESTROMP N R LUNDEGAARD L F,STAPPEN F N,MOSSIN S,BEATO P,BORDIGA S,LAMBERTI C.Characterization of Cu-exchanged SSZ-13:A comparative FT-IR,UV-Vis and EPR study w ith Cu-ZSM-5 and Cu-beta w ith similar Si/Al and Cu/Al ratios[J].Dalton Trans,2013,42(35):12741-12761.
[45]ISMAGILOV Z R,YASHNIK S A,ANUFRIENKO V F,LARINA T V,VASENIN N T,BULGAKOV N N,VOSELET S V,TSYKOZAL T.Linear nanoscale clusters of CuO in Cu-ZSM-5 catalysts[J].Appl Surf Sci,2004,226(1/3):88-93.
[46]KIMMH,NAMI-S,KIMY G.Characteristics of mordenite-type zeolite catalysts deactivated by SO2for the reduction of NO w ith hydrocarbons[J].J Catal,1998,179(2):350-360.
[47]CHADWICK D,HASHEMI T.Adsorbed corrosion inhibitors studied by electron spectroscopy:Benzotriazole on copper and copper alloys[J].Corros Sci,1978,18(1):39-51.
[48]GONG J L,YUE H R,ZHAO Y J,ZHAO S,ZHAO L,LV J,WANG S P,MA X B.Synthesis of ethanol via syngas on Cu/SiO2catalysts w ith balanced Cu0-Cu+sites[J].J Am Chem Soc,2012,134(34):13922-13925.
[49]GUO H J,ZHANG H R,PENG F,YANG H J,XIONG L,WANG C,HUANG C,CHEN X D,MA L L.Effects of Cu/Fe ratio on structure and performance of attapulgite supported CuFeCo-based catalyst for mixed alcohols synthesis from syngas[J].Appl Catal A:Gen,2015,503(25):51-61.
[50]LI F,ZHANG L H,EVANS D G,DUAN X.Structure and surface chemistry of manganese-doped copper-based mixed metal oxides derived from layered double hydroxides[J].Colloids Surf A,2004,244(1/3):169-177.
[51]DATKA J,TUREK A M,JEHNG J M,WACHS I E.Acidic properties of supported niobium oxide catalysts:An infrared spectroscopy investigation[J].J Catal,1992,135(1):186-199.
[52]BARZETTI T,SELLI E,MOSCOTTI D,FORNI L.Pyridine and ammonia as probes for FT-IR analysis of solid acid catalysts[J].J Chem Soc Faraday Trans,1996,92(8):1401-1407.
[53]SULTANA A,HANEDA M,FUJITANI T,HAMADA H.Influence of Al2O3support on the activity of Ag/Al2O3catalysts for SCR of NOw ith decane[J].Catal Lett,2007,114(1/2):96-102.
[54]CHMIELARZ L,PIWOWARSKA Z,KU'S TROWSKI P,WEGRZYN A,GIL B,KOWALCZYK A,DUDEK B,DZIEMBAJ R,MICHALIKET M.Comparison study of titania pillared interlayered clays and porous clay heterostructures modified w ith copper and iron as catalysts of the DeNOxprocess[J].Appl Clay Sci,2011,53(2):164-173.
[55]LONG R Q,YANG R T.Selective catalytic reduction of nitrogen oxides by ammonia over Fe3+-Exchanged TiO2-pillared clay catalysts[J].JCatal,1999,186(2):254-268.
[56]EMEIS C A.Determination of integrated molar extinction coefficients for infrared absorption bands of pyridine absorbed on solid acid catalysts[J].J Catal,1993,141(2):347-354.
[57]LI J H,ZHU Y Q,KE R,HAO J M.Improvement of catalytic activity and sulfur-resistance of Ag/TiO2-Al2O3for NO reduction w ith propene under lean burn conditions[J].Appl Catal B:Environ,2008,80(3/4):202-213.
[58]DATKA J,GIL B,KUBACKA A.Heterogeneity of OH groups in H-mordenites:Effect of dehydroxylation[J].Zeolites,1996,17(5/6):428-433.
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