袁亚梅,陈慧,赵丹阳,吴驰,耿皎,沈俭一.硫化镍和磷化镍的HDS加氢活性和稳定性[J].分子催化编辑部,2021,35(3):263-272
硫化镍和磷化镍的HDS加氢活性和稳定性
Stability and Activity of Ni2P and NiSx for the Hydrotreating Reactions
投稿时间:2020-11-08  修订日期:2021-01-13
DOI:10.16084/j.issn1001-3555.2021.03.007
中文关键词:  Ni2P/Al2O3催化剂  NiSx/Al2O3催化剂  PPh3液相磷化  CS2液相硫化  物相稳定性  加氢精制反应
英文关键词:Ni2P/Al2O3 catalyst  NiSx/Al2O3 catalyst  liquid phase phosphidation by PPh3  liquid phase sulfidation by CS2  phase stability  hydrotreating reaction
基金项目:本工作受到国家自然科学基金面上项目(21773108)、国家自然科学基金中德合作项目(21761132006)和中央高校基本科研业务费资助
作者单位E-mail
袁亚梅 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023  
陈慧 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023  
赵丹阳 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023  
吴驰 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023  
耿皎 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023  
沈俭一 南京大学 化学化工学院 介观化学教育部重点实验室, 江苏 南京 210023 jyshen@nju.edu.cn 
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中文摘要:
      采用共沉淀法制备了高分散80% Ni/Al2O3催化剂,经350℃焙烧,得高分散NiO/Al2O3(NiO粒径~3 nm),将其以CS2硫化(310℃,4 h)或PPh3磷化(320℃,36 h),分别获得了高分散的硫化镍(Ni3S2和Ni3S4,5.8 nm)和Ni2P(7.0 nm),在二苯并噻吩(DBT)的加氢脱硫(HDS)反应中,Ni2P的活性远高于NiSx(360℃时DBT的转化率分别为100%和75%).若将NiSx用PPh3磷化,则NiSx全部转化为Ni2P(13.3 nm),其HDS活性远高于原来的NiSx且与直接磷化获得的Ni2P(7.0 nm)相当.反之,若将Ni2P用CS2硫化,则Ni2P物相不变,粒径也没有长大,表明Ni2P物相远比NiSx稳定,且其HDS活性高于直接磷化的Ni2P,表明其Ni2P表面可能生成了HDS活性更高的某种Ni-P-S物种.
英文摘要:
      A highly dispersed 80% Ni/Al2O3 catalyst was prepared by the co-precipitation method, which was calcined in air at 350 ℃ to obtain a highly dispersed NiO/Al2O3 with NiO particles of about 3 nm. The NiO/Al2O3 was then sulfided with CS2 at 310 ℃ to nickel sulfides (Ni3S2 and Ni3S4 of about 5.8 nm), or phosphided with PPh3 at 320 ℃ to Ni2P (7.0 nm). The NiSx phases were completely converted into Ni2P (13.3 nm) when phosphided with PPh3 at 320 ℃, which was as active as the directly phosphided Ni2P (7.0 nm). In contrast, the phase and crystalline size of Ni2P did not change when treated with CS2 even at 360 ℃, indicating that the Ni2P was much more stable than the NiSx (Ni3S2 and Ni3S4). Moreover, the Ni2P/Al2O3 treated with CS2 at 310 ℃ was more active than the directly phosphided Ni2P for the hydrodesulfication (HDS) reaction, indicating that the incorporation of S into Ni2P might generate some Ni-P-S species that were more active than the Ni-P surface species for the HDS reactions.
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