燃料化学学报
燃料化學學報
연료화학학보
JOURNAL OF FUEL CHEMISTRY AND TECHNOLOGY
2014年
9期
1111-1118
,共8页
束韫%张凡%王洪昌%朱金伟
束韞%張凡%王洪昌%硃金偉
속운%장범%왕홍창%주금위
氧化铈%氧化钛%堇青石%脱硝%氨选择催化还原%抗硫抗水性
氧化鈰%氧化鈦%堇青石%脫硝%氨選擇催化還原%抗硫抗水性
양화시%양화태%근청석%탈초%안선택최화환원%항류항수성
CeO2%TiO2%cordierite%denitration%selective catalytic reduction of NOx%SO2 and H2 O resistance
采用浸渍法制备了以堇青石为基底、氧化铈为活性组分的整体式脱硝催化剂CeO2/TiO2/堇青石催化剂。通过与商业钒基催化剂( V2 O5-WO3/TiO 2/堇青石)的对比研究发现, CeO2/TiO2/堇青石催化剂表现出了优良的抗硫抗水性能,经过30 h抗硫抗水实验,CeO2/TiO2/堇青石催化剂的氮氧化物转化率仍能保持在70%以上,仅下降了5%。 BET、XRD、FT-IR和TG表征结果表明,在含硫含水气氛中反应时,CeO2/TiO2/堇青石和V2 O5-WO3/TiO2/堇青石催化剂表面均有硫酸铵盐的生成,且前者的生成量明显低于后者。N H3-DRIFT分析结果表明,在含硫含水气氛中两种催化剂表面Br?nsted酸性都被增强,而Lewis酸性有所减弱。进一步的XPS分析结果表明,烟气中的SO2+H2O 会使催化剂表面Ce4+向Ce3+发生转化,从而导致化学吸附氧含量增加,这是CeO2/TiO2/堇青石催化剂具有优良抗硫抗水性能的重要原因。
採用浸漬法製備瞭以堇青石為基底、氧化鈰為活性組分的整體式脫硝催化劑CeO2/TiO2/堇青石催化劑。通過與商業釩基催化劑( V2 O5-WO3/TiO 2/堇青石)的對比研究髮現, CeO2/TiO2/堇青石催化劑錶現齣瞭優良的抗硫抗水性能,經過30 h抗硫抗水實驗,CeO2/TiO2/堇青石催化劑的氮氧化物轉化率仍能保持在70%以上,僅下降瞭5%。 BET、XRD、FT-IR和TG錶徵結果錶明,在含硫含水氣氛中反應時,CeO2/TiO2/堇青石和V2 O5-WO3/TiO2/堇青石催化劑錶麵均有硫痠銨鹽的生成,且前者的生成量明顯低于後者。N H3-DRIFT分析結果錶明,在含硫含水氣氛中兩種催化劑錶麵Br?nsted痠性都被增彊,而Lewis痠性有所減弱。進一步的XPS分析結果錶明,煙氣中的SO2+H2O 會使催化劑錶麵Ce4+嚮Ce3+髮生轉化,從而導緻化學吸附氧含量增加,這是CeO2/TiO2/堇青石催化劑具有優良抗硫抗水性能的重要原因。
채용침지법제비료이근청석위기저、양화시위활성조분적정체식탈초최화제CeO2/TiO2/근청석최화제。통과여상업범기최화제( V2 O5-WO3/TiO 2/근청석)적대비연구발현, CeO2/TiO2/근청석최화제표현출료우량적항류항수성능,경과30 h항류항수실험,CeO2/TiO2/근청석최화제적담양화물전화솔잉능보지재70%이상,부하강료5%。 BET、XRD、FT-IR화TG표정결과표명,재함류함수기분중반응시,CeO2/TiO2/근청석화V2 O5-WO3/TiO2/근청석최화제표면균유류산안염적생성,차전자적생성량명현저우후자。N H3-DRIFT분석결과표명,재함류함수기분중량충최화제표면Br?nsted산성도피증강,이Lewis산성유소감약。진일보적XPS분석결과표명,연기중적SO2+H2O 회사최화제표면Ce4+향Ce3+발생전화,종이도치화학흡부양함량증가,저시CeO2/TiO2/근청석최화제구유우량항류항수성능적중요원인。
A monolithic CeO2/TiO2/cordierite deNOx catalyst was prepared by an impregnation method, with cordierite as the substrate and CeO2 as the active component.The CeO2/TiO2/codr ierite catalyst exhibits exceleln t resistance against SO2 and H2 O in the selective catayl tic reduction ( SCR) of NOx with NH3 , compared with the commercial vanadium-based catalyst ( V2 O5-WO3/TiO2/cordierite);the CeO2/TiO2/cordierite catalyst gives a conversion of NOxa bove 70%after 30h rse istance test ga ainst SO2+H2 O,o nly declined by 5%.BET, XRD, FT-IR and TG reslu ts indicated that ammonium sulfate is formed on the surface of both CeO2/TiO2/c ordierite and V2 O5-WO3/TiO2/corid erti e caat yl stsdu ring the SCR reaction in the presence of SO2 and H2 O, but on the former, the amount of ammonui m sulfate deposited is much less.NH3-DR IFT results us ggested that the surface Br?nsted acidity is strengthened, whereas the surface Lewis acidity is weakened during the SCR reaction in the presence of SO2 and H2 O.XPS results further displayed that SO2+H2 O in flue gas may induce a reduction of Ce from Ce4+to Ce3+on CeO2/TiO2/cordierite catalyst, resulting in an increase of th e chemisorbed oxygen amount, which contributes to the excellent resistance of the CeO2/TiO2/cordierite catalysta gainst SO2 and H2 O during the SCR reaction.