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[1]孙炜,王鹏,杨犁,等.二苯并噻吩加氢脱硫过程在镍钼硫催化剂表面的吸附[J].武汉工程大学学报,2013,(02):51-56.[doi:103969/jissn16742869201302011]
　SUN Wei,WANG Peng,YANG Li,et al.Adsorption of dibenzothiophene hydrodesulfurization process over NiMoS Catalyst[J].Journal of Wuhan Institute of Technology,2013,(02):51-56.[doi:103969/jissn16742869201302011]
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二苯并噻吩加氢脱硫过程在镍钼硫催化剂表面的吸附(/HTML)
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《武汉工程大学学报》[ISSN:1674-2869/CN:42-1779/TQ]

卷:
期数:
2013年02期
页码:
51-56
栏目:
化学与化学工程
出版日期:
2013-02-28

文章信息/Info

Title:
Adsorption of dibenzothiophene hydrodesulfurization process over NiMoS Catalyst
文章编号:
16742869(2013)02005106
作者:
孙炜; 王鹏; 杨犁; 方元
武汉工程大学绿色化工过程教育部重点实验室,湖北 武汉 430074
Author(s):
SUN Wei; WANG Peng; YANG Li; FANG Yuan
Key Laboratory for Green Chemical Process of Ministry of Education, Wuhan Institute of Technology, Wuhan 470074, China
关键词:
二苯并噻吩; 加氢脱硫; 密度泛函理论; 量子化学
Keywords:
dibenzothiophene;  hydrodesulfurization;  density functional theory;  quantum chemisty
分类号:
TQ015
DOI:
103969/jissn16742869201302011
文献标志码:
A
摘要:
二苯并噻吩（DBT）作为石油中最难脱除的含硫组分之一，对其加氢脱硫(HDS)过程的研究有着十分重要的意义.针对二苯并噻吩在加氢脱硫过程中各含硫物质在镍钼硫（NiMoS）催化剂表面吸附情况，采用量子化学中密度泛函理论方法，计算了二苯并噻吩（DBT）、四氢二苯并噻吩（4H—DBT）、六氢二苯并噻吩（6H—DBT）和十二氢二苯并噻吩（HY—DBT）等四种含硫物质于NiMoS催化剂表面上吸附能.主要研究垂直吸附和平行吸附两种吸附方式，研究结果表明，各含硫化合物在NiMoS催化剂表面上的吸附过程都是放热过程.当DBT、4H—DBT、6H—DBT和HY—DBT四种硫化物垂直吸附于催化剂表面，此时形成稳定构象，且各体系吸附能逐渐增大；而当各硫化物平行吸附时，各体系吸附能呈减小的趋势.其中DBT在催化剂表面吸附时，垂直吸附形式和平面吸附形式可能同时存在，而4H—DBT、6H—DBT和HY—DBT三种含硫物质则更易以垂直吸附形式吸附于催化剂表面.同时DBT、4H—DBT、6H—DBT和HY—DBT在NiMoS催化剂上吸附能较硫化钼（MoS2）催化剂更低.
Abstract:
Dibenzothiophene (DBT)is a difficult removal sulfur compound in the petroleum, whose hydrodesulfurization (HDS) process studies have great significance. The surface adsorption of DBT and its hydrogenation sulfur compounds were studied on NiMoS catalyst surface during hydrodesulfurization (HDS) process. The surface adsorbed energies of Dibenzothiophene (DBT), tetrahydrodibenzothiophene (4H—DBT), hexahydrodibenzothiophene (6H—DBT), and completely hydrogenated dibenzothiophene (HY—DBT) were computed based on density functional theory in quantum chemistry. Two different adsorbed configurations as perpendicular and flat adsorptions, were studied. The results show that it is an exothermic process for the adsorption process of DBT and its hydrogenation sulfur compounds on NiMoS catalyst surface. The stable configurations are obtained when DBT, 4H—DBT, 6H—DBT and HY—DBT are perpendicular absorbted on the surface of catalyst, at same time their adsorption energies are grown up by increasing of the hydrgen atoms; the opposite results are got when they are flat absorbted on the surface of catalyst. And then there are both perpendicular and flat adsorptions for DBT on the surface of NiMoS catalyst, but the others sulfur compounds such as 4H—DBT, 6H—DBT and HY—DBT are easier perpendicular adsorbed on NiMoS catalyst surface. Meanwhile the adsorption energies on the surface of NiMoS catalyst are lower than the the surface of MoS2 catalyst.

参考文献/References:

［1］钱松.世界原油质量及我国面临的挑战\[J\]. 中国石油和化工, 2005,(6):4550.［2］王天普. 石油化工清洁生产与环境保护技术进展\[M\]. 北京:中国石油出版社, 2006:35.［3］徐永强，赵瑞玉，商红岩，等.二苯并噻吩和4-甲基二苯并噻吩在Mo和CoMo/γ-Al2O3催化剂上加氢脱硫反应机理\[J\]. 石油学报(石油加工), 2003,19(5):1421.［4］Wang A, Wang Y, Kabe T, et al. Hydrodesulfurization of Dibenzothiophene over Siliceous MCM41Supported Catalysts: I. Sulfided CoMo Catalysts \[J\]. J Catal, 2001,199:1929.［5］Nag N K，Sapre A V，Brodefick D H，et al．Hydrodesulfurization of polycyclic aromaticscatalyzed by sulfided CoMo/Al2O3：The relative reactivities \[J\]．J Catal，1979，57:509512．［6］Yang H, Fairbridge C, Ring Z. Adsorption of Dibenzothiophene Derivatives over a MoS2 NanoclusterA Density Functional Theory Study of StructureReactivity Relations \[J\]. Energy Fuels, 2003,17:387398.［7］Grange P, Vanhaeren X, Hydrotreating catalysts, an old story with new challenges \[J\]. Catal Today, 1997,36(4):375391.［8］Schweiger H , Raybaud P, Toulboat H. Promoted sensitive shapes of co(ni)mos nanocatalysts in sulforeductive conditions \[J\]. J Catal, 2002,212(1):3338.［9］Sun M, Nelson A E, Adjaye J. On the incorporation of nickel and cobalt into MoS2edge structures \[J\]. J Catal, 2004,226(1):3240.［10］曹斌,高金森,徐春明.分子模拟技术在石油相关领域的应用\[J\]. 化学进展, 2004,16(2):291298.［11］居沈贵，曾永平，姚虎卿，等.吸附脱硫及分子模拟应用的研究进展\[J\]. 现代化工, 2005,25(7):1113.［12］石灵娟，周涵，代振宇.几种典型硫化物在MoS2晶面上的吸附形式研究\[J\]. 计算机与应用化学, 2004,21(3):501504.［13］叶天旭，徐永强，张予辉，等.Co/MoS2催化剂加氢脱硫活性的量子化学研究\[J\]. 石油大学学报：自然科学版, 2005,29(4):5157.［14］Kahe T, Qian W, Ishihara A. Mechanism of hydrodesulfurization of hydrogenation on CoMo/Al2O3 and Co/Al2O3 catalyst by the use of radioisotope 35S tracer \[J\]. J Catal，1993,143:239248.［15］Michaud P, Lemberton J L, Perot G. Hydrosulfurization of dibenzothiophene and 4,6dimethyldibenzothiophene: Effect of an acid component on the activity of a sulfided NiMo on adumina catalyst \[J\]. Appl Catal A, 1998,169:343353. ［16］Nicholson D E. Identification of Adsorption Species by Infrared Spectrometry: ThiopheneCobalt Moly bdateMolybdenum Sulfide System \[J\]. Anal Chem, 1962,34(3):370374.［17］Ma X, Schobert H H. Molecular simulation on hydrodesulfurization of thiophenic compounds over MoS2 using ZINDO \[J\]. J Catal, 2000,160:409427.［18］Ma X, Schobert H H. Hydrodesulfurization of thiophenic compounds on MoS2: A computational Study Using Zindo \[J\]. Preper Div Fuel Chem ACS. 1997,42(3):657661.［19］Whitehurst D, Isoda T, Mochida I. Present State of the Art and Future Challenges in the Hydrodesulfurization of Polyaromatic Sulfur Compounds \[J\]. J Catal, 1998,42:345471.［20］Devanneaux J, Maurin J. Hydrodesulfurization and hydrogenation of thiophenic compounds on a CoMo/Al/sub 2/O/sub 3/catalyst.\[J\]. J Catal, 1981,69:202205.［21］Orita H, Uchida K, Itoh N. A volcanotype relationship between the energy of thiophene on promoted MoS2 clustermodel catalysts and the experimental HDS activity: ab initio density functional study \[J\]. Appl Catal A, 2004,258(1):115120.

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备注/Memo

备注/Memo:
收稿日期：20121021基金项目：国家自然科学基金（No.50576028）；湖北省教育厅重点项目（No.D20081508）作者简介：孙炜（1967），男，湖北武汉人，教授，博士，硕士研究生导师.研究方向：分子模拟.
更新日期/Last Update: 2013-04-16