石油学报（石油加工）
石油學報（石油加工）
석유학보（석유가공）
Acta Petrolei Sinica (Petroleum Processing Section)
2015年
5期
1042-1047
,共6页
张孔远%昃彬%张唯稚%王宗波%刘晨光
張孔遠%昃彬%張唯稚%王宗波%劉晨光
장공원%측빈%장유치%왕종파%류신광
加氢脱硫催化剂%乙二醇%磷酸%配合物
加氫脫硫催化劑%乙二醇%燐痠%配閤物
가경탈류최화제%을이순%린산%배합물
hydrodesulfurization catalyst%ethylene glycol%phosphate%complex
在CoMoP共浸渍液中加入乙二醇（EG）制备CoMoP‐EG／γ‐Al2O3系列催化剂。采用 UV‐Vis、 TG／DTG、FT‐IR、低温N2吸附、H2‐TPR、HRTEM 等手段对其进行表征，并以直馏柴油为原料，采用高压微反装置评价催化剂的加氢脱硫和加氢脱氮活性。结果表明，浸渍液中的乙二醇未与活性金属离子形成新的配合物。乙二醇与载体发生相互作用形成Al—O—C键，减弱了活性组分与载体的相互作用，提高了活性组分的分散性。与未加乙二醇制备的硫化态CoMoP／γ‐Al2 O3相比，硫化态CoMoP‐EG／γ‐Al2 O3催化剂中MoS2晶粒的堆垛层数增加，片层长度减少，有利于Ⅱ型Co—M o—S活性相的形成。在反应温度350℃、氢分压6.0 M Pa、空速1.5 h－1、氢／油体积比400条件下，采用最佳乙二醇加入量制备的CoMoP‐EG／γ‐Al2 O3催化剂，可使直馏柴油的硫质量分数由13298μg／g降至6μg／g ，氮质量分数由169.7μg／g降至0.4μg／g。
在CoMoP共浸漬液中加入乙二醇（EG）製備CoMoP‐EG／γ‐Al2O3繫列催化劑。採用 UV‐Vis、 TG／DTG、FT‐IR、低溫N2吸附、H2‐TPR、HRTEM 等手段對其進行錶徵，併以直餾柴油為原料，採用高壓微反裝置評價催化劑的加氫脫硫和加氫脫氮活性。結果錶明，浸漬液中的乙二醇未與活性金屬離子形成新的配閤物。乙二醇與載體髮生相互作用形成Al—O—C鍵，減弱瞭活性組分與載體的相互作用，提高瞭活性組分的分散性。與未加乙二醇製備的硫化態CoMoP／γ‐Al2 O3相比，硫化態CoMoP‐EG／γ‐Al2 O3催化劑中MoS2晶粒的堆垛層數增加，片層長度減少，有利于Ⅱ型Co—M o—S活性相的形成。在反應溫度350℃、氫分壓6.0 M Pa、空速1.5 h－1、氫／油體積比400條件下，採用最佳乙二醇加入量製備的CoMoP‐EG／γ‐Al2 O3催化劑，可使直餾柴油的硫質量分數由13298μg／g降至6μg／g ，氮質量分數由169.7μg／g降至0.4μg／g。
재CoMoP공침지액중가입을이순（EG）제비CoMoP‐EG／γ‐Al2O3계렬최화제。채용 UV‐Vis、 TG／DTG、FT‐IR、저온N2흡부、H2‐TPR、HRTEM 등수단대기진행표정，병이직류시유위원료，채용고압미반장치평개최화제적가경탈류화가경탈담활성。결과표명，침지액중적을이순미여활성금속리자형성신적배합물。을이순여재체발생상호작용형성Al—O—C건，감약료활성조분여재체적상호작용，제고료활성조분적분산성。여미가을이순제비적류화태CoMoP／γ‐Al2 O3상비，류화태CoMoP‐EG／γ‐Al2 O3최화제중MoS2정립적퇴타층수증가，편층장도감소，유리우Ⅱ형Co—M o—S활성상적형성。재반응온도350℃、경분압6.0 M Pa、공속1.5 h－1、경／유체적비400조건하，채용최가을이순가입량제비적CoMoP‐EG／γ‐Al2 O3최화제，가사직류시유적류질량분수유13298μg／g강지6μg／g ，담질량분수유169.7μg／g강지0.4μg／g。
CoMoP‐EG/γ‐Al2 O3 catalysts were prepared by adding ethylene glycol (EG ) to the CoMoP co‐impregnation solutions and characterized by means of UV‐Vis ,TG/DTG ,FT‐IR ,BET , H2‐TPR , HRTEM . The HDS and HDN performances of prepared CoMoP‐EG/γ‐Al2 O3 were evaluated in a high pressure microreactor with straight‐run diesel as feed .The results indicated that there was not any new Co or Mo complex formed in co‐impregnation solution when ethylene glycol was added .Ethylene glycol could interact with γ‐Al2 O3 to form Al—O—C bond ,weakening the interaction between metals and supports and promoting the dispersion of metals on the surface of supports .Compared to sulfide CoMoP/γ‐Al2 O3 ,the stacking number of MoS2 particles in sulfide CoMoP‐EG/γ‐Al2 O3 increased and the MoS2 slab length decreased , facilitating the formation of Co—Mo—S active phases of type Ⅱ .At the reaction conditions of θ=350℃ ,p(H2 )= 6.0 MPa , V (H2 )/V (Oil)=400 ,LHSV = 1.5 h-1 and with the CoMoP‐EG/γ‐Al2 O3 of optimum ethylene glycol amount as catalyst ,the sulfur and nitrogen mass fractions of straight‐run diesel feedstock could be reduced from 13298 to 6 μg/g and from 169.7 to 0.4 μg/g ,respectively .
