燃料化学学报
燃料化學學報
연료화학학보
JOURNAL OF FUEL CHEMISTRY AND TECHNOLOGY
2014年
7期
833-838
,共6页
冯军鹏%张晔%吕占军%李学宽
馮軍鵬%張曄%呂佔軍%李學寬
풍군붕%장엽%려점군%리학관
二甲基二硫醚%Ni/ Al2 O3%加氢反应%失活机理
二甲基二硫醚%Ni/ Al2 O3%加氫反應%失活機理
이갑기이류미%Ni/ Al2 O3%가경반응%실활궤리
dimethyl disulfide%Ni/Al2 O3%hydrogenation%poison
考察了二甲基二硫醚(CH3 SSCH3)对 Ni/ Al2 O3催化剂上苯、环己烯和苯乙烯加氢活性的影响,并采用 BET、XRD、H-TPR、XPS、SEM 和 EA 等手段对催化剂进行表征。实验结果表明,在 CH3 SSCH3存在下,Ni/ Al2 O3催化剂对苯和环己烯加氢迅速失活,且环己烯加氢对 CH3 SSCH3的耐硫性要略强于苯加氢,而苯乙烯中共轭烯烃的加氢转化率则维持100%长时间不变。 CH3 SSCH3的影响顺序为芳环>单烯烃>共轭烯烃。此外,通过设计实验研究了 CH3 SSCH3对催化剂的毒化机理,发现CH 23 SSCH 3分子首先吸附在催化剂的表面,并发生氢解生成甲烷随尾气逸出,故 CH3 SSCH3分子中碳对催化剂的失活影响较小,而留下的硫原子则与镍活性组分发生相互作用,毒化催化剂。
攷察瞭二甲基二硫醚(CH3 SSCH3)對 Ni/ Al2 O3催化劑上苯、環己烯和苯乙烯加氫活性的影響,併採用 BET、XRD、H-TPR、XPS、SEM 和 EA 等手段對催化劑進行錶徵。實驗結果錶明,在 CH3 SSCH3存在下,Ni/ Al2 O3催化劑對苯和環己烯加氫迅速失活,且環己烯加氫對 CH3 SSCH3的耐硫性要略彊于苯加氫,而苯乙烯中共軛烯烴的加氫轉化率則維持100%長時間不變。 CH3 SSCH3的影響順序為芳環>單烯烴>共軛烯烴。此外,通過設計實驗研究瞭 CH3 SSCH3對催化劑的毒化機理,髮現CH 23 SSCH 3分子首先吸附在催化劑的錶麵,併髮生氫解生成甲烷隨尾氣逸齣,故 CH3 SSCH3分子中碳對催化劑的失活影響較小,而留下的硫原子則與鎳活性組分髮生相互作用,毒化催化劑。
고찰료이갑기이류미(CH3 SSCH3)대 Ni/ Al2 O3최화제상분、배기희화분을희가경활성적영향,병채용 BET、XRD、H-TPR、XPS、SEM 화 EA 등수단대최화제진행표정。실험결과표명,재 CH3 SSCH3존재하,Ni/ Al2 O3최화제대분화배기희가경신속실활,차배기희가경대 CH3 SSCH3적내류성요략강우분가경,이분을희중공액희경적가경전화솔칙유지100%장시간불변。 CH3 SSCH3적영향순서위방배>단희경>공액희경。차외,통과설계실험연구료 CH3 SSCH3대최화제적독화궤리,발현CH 23 SSCH 3분자수선흡부재최화제적표면,병발생경해생성갑완수미기일출,고 CH3 SSCH3분자중탄대최화제적실활영향교소,이류하적류원자칙여얼활성조분발생상호작용,독화최화제。
Poisoning effect of dimethyl disulfide ( CH3 SSCH3 ) on Ni/Al2 O3 catalysts for hydrogenation of benzene, cyclohexene and styrene was studied. The structures and properties of the catalysts were investigated by means of BET, XRD, H2-TPR, XPS, SEM and EA. Results indicated that with the existence of CH3 SSCH3 , Ni/Al2 O3 catalysts quickly deactivated for benzene and cyclohexene hydrogenation, while the activity for styrene hydrogenation remained well. The sulfur tolerance of Ni/Al2 O3 catalysts for cyclohexene hydrogenation was little better than that of benzene hydrogenation. The conversion of conjugated double bond of styrene can keep 100% for a long time. For hydrogenation reactions, the poisoning effects of CH3 SSCH3 over Ni/Al2 O3 were in the order of aromatic nucleus>monoene>conjugated alkene. In addition, poisoning mechanism of CH3 SSCH3 for Ni/Al2 O3 catalyst was also discussed. CH3 SSCH3 molecules were firstly adsorbed on the surface of catalyst and then dissociated to CH4 under the function of hydrogen and catalyst. It is concluded that the toxicity of carbon in CH3 SSCH3 for catalysts isneglectful and remaining sulfur is the dominant poisoning factor by the interaction with active component.