Al-PILC负载铜铁复合氧化物在NH_3选择性催化还原NO中的协同作用  

Synergetic effect of Cu-Fe composite oxides supported on Al-PILC for SCR of NO with NH_3

作　　者：朱斌[1] 费兆阳[1,2] 陈献[1] 汤吉海[1] 崔咪芬[1] 乔旭[1,2] 

机构地区：[1]南京工业大学化学化工学院,江苏南京210009 [2]南京工业大学材料化学工程国家重点实验室,江苏南京210009

出　　处：《燃料化学学报》2014年第9期1102-1110,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21306089);国家科技支撑计划(2011BAE18B01);江苏省高校自然科学基金(13KJB530006);江苏省科技支撑计划(BE2011830)

摘　　要：以铝柱撑黏土（Al-PILC）为载体采用旋蒸-浸渍法制备了铜、铁单组分催化剂（Cu/Al-PILC、Fe/Al-PILC）和铜铁复合氧化物催化剂（CuFe/Al-PILC），并测试其对NH3选择性催化还原NO反应（NH3-SCR）的催化性能。相比Cu/Al-PILC和Fe/Al-PILC，CuFe/Al-PILC活性组分之间有较强的协同效应，显著提高了催化剂的脱硝性能。CuFe/Al-PILC在290～450℃的宽温区NO脱除效率保持90％以上，最高可达97％。此外，CuFe/Al-PILC有很好的抗水抗硫性能，催化活性不受反应气氛中水蒸气和SO2的影响。XRD、UV-vis、XPS和N2吸附脱附表征结果表明，CuFe/Al-PILC中活性组分相互作用生成CuFe2O4，有利于活性组分在载体表面分散，提高催化剂的比表面积和孔容；H2-TPR表征结果表明，CuFe/Al-PILC活性组分在载体表面生成的CuFe2O4改善了催化剂氧化还原性能，有利于NH3对NO选择性的还原；NH3-TPD表征结果表明，CuFe/Al-PILC在较宽温区范围内对NH3都有很好的吸附，这有利于提高催化剂表面还原物种的浓度，从而保证催化剂在较宽温区范围内具有较好的NO脱除效率。Cu/Al-PILC, Fe/Al-PILC and CuFe/Al-PILC were prepared by rotary evaporation-impregnation method using Al-PILC as support.Selected catalytic reduction of NO with NH3（ NH3-SCR） was carried out in a fixed bed er actor to evaluate their catalytic performance.Compared to Cu/Al-PILC and FeA/l-PILC, CuFe/Al-PILC showed better NO removal efficiency （ 97%） and a wider temperature range （ 290 -450℃） of 90%DeNO because of the strong synergetic effect of Cu-Fe com pso tie oxides.Moreover, CuFe/Al-PILC showed good resistance to water vapor and SO2 .XRD, UV-vis, XPS and N2 adsorption were used to characterize the structure of the catalysts.A new phase CuFe2 O4 formed in CuF e/Al-PILC, which changed the surface properties of CuFe/Al-PILC, improved the dispersion of Cu and Fe on the Al-PILC surface and increased ABET and vp of CuFe/Al-PILC.H2-TPR confirmed the existence of CuFe2 O4 , which improved the re-dox property of CuFe/Al-PILC.The result of NH3-TPD implied that the surface acidity of CuFe/Al-PILC made it possible to adsorb and desorb NH3 in a wide temperature range.The concentration of reducible species on the surface of CuFe/Al-PILC increased, which resulted in high NO removal efficiency.

关 键 词：选择性还原 脱硝 铝柱撑黏土 铜铁复合催化剂 协同作用 

分 类 号：I643.3[文学—其他各国文学]