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MoO_3-LaHY催化剂的固相反应制备及其加氢脱硫性能研究 被引量:2

Hydrodesulfurization performance of MoO_3-LaHY catalyst prepared by solid-state reaction
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摘要 在空气气氛中由钼酸铵和LaHY分子筛固相反应制备了MoO3-LaHY催化剂,用XRD和NH3-TPD对其进行了表征,并以二苯并噻吩/正癸烷溶液为模型反应物(二苯并噻吩的质量分数为0.6%),评价了MoO3-LaHY的加氢脱硫催化性能。结果表明,在520℃下进行固相反应制备催化剂时,4.36%的Mo物种可借助固相反应进入到分子筛的体相形成单相复合体nMoOx.LaHY,剩余的Mo物种仍以MoO3的形式分散在分子筛外表面。由于单相复合体的形成,催化剂的晶胞参数增大,酸量有所下降。硫化处理后得到的硫化态MoO3-LaHY催化剂在310℃、4.0MPa、反应空速为20h-1的条件下进行加氢脱硫时,二苯并噻吩转化率达到了86.74%。随固相反应温度的升高,所制备的催化剂中Mo物种进入LaHY体相中的量有所增大,但其硫化态催化剂的二苯并噻吩加氢脱硫活性的变化幅度并不大。 MoOx-LaHY catalysts were prepared with the mixture of(NH4)6Mo7O24·4H2O and LaHY through solid-state reaction under air atmosphere and characterized by XRD and NH3-TPD techniques;their hydrodesulfurization(HDS) performance was evaluated by using the solution of dibenzothiophene(DBT,0.6% by mass) in decane as a model reactant.The results indicated that by using solid-state reaction at 520℃,4.36% of Mo species is incorporated into the molecular sieve LaHY,which forms the single-phase complex nMoOx·LaHY,while the rest Mo species is dispersed on the outer surface of LaHY.As a result of forming the single-phase complex,the lattice parameters of MoOx-LaHY catalysts are enlarged and their acidity is reduced.Over the sulfided MoOx-LaHY catalysts,the conversion of DBT reaches 86.74% for the HDS under the conditions of 310℃,4.0MPa and a space velocity 20h-1.Raising the solid-state reaction temperature may increase the content of the single-phase complex incorporated in the resultant MoOx-LaHY catalysts,but it cannot significantly enhance their HDS activity.
出处 《燃料化学学报》 EI CAS CSCD 北大核心 2011年第7期538-542,共5页 Journal of Fuel Chemistry and Technology
基金 中国石油科技创新基金(2009D-5006-04-03)
关键词 固相反应 单相复合体 表征 二苯并噻吩 加氢脱硫 solid-state reaction single-phase complex characterization dibenzothiophene hydrodesulfurization
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参考文献14

  • 1SONG C S, MAX L. New design approaches to ultra-clean diesel fuels by deep desulfurization and deep dearomatization [ J ]. Appl Catal B, 2003, 41 ( 2 ) : 207-238.
  • 2LI X, WANG A J, PRINS R. Kinetics of HDS of 4,6-dimethyldibenzothiophene and its hydrogenated intermediates over sulfided Mo and NiMo on γ/-AI203 [J]. J Catal, 2007, 250(2) : 283-293.
  • 3RALPH T Y, ARTURO J H, FRANCES H Y. Desulfurization of transportation fuels with zeolites under ambient conditions[J]. Science, 2003, 301(5629): 79-81.
  • 4ABU 1 I, SMITH K J. Hydrodenitrogenation of carbazole over a series of bulk NixMoP catalysts[ J]. Catal Today, 2007, 125 (4) : 248-255.
  • 5ARTURO J H, QI G S, YANG R T. Desulfurization of commercial fuels by ~r-complexation: Monolayer CuCI/γ-A1203 [ J]. Appl Catal B. 2005, 61(3) : 212-218.
  • 6李大东.21世纪的炼油技术与催化[J].石油学报(石油加工),2005,21(3):17-24. 被引量:69
  • 7TURAGA U T, MA X L, SONG C S. Influence of nitrogen compounds on deep hydrodesulfurization of 4,6-dimethyldibenzothiophene over A12O3- and MCM-41-supported Co-Mo sulfide catalysts[ J].Catal Today, 2003, 86(4) : 265-275.
  • 8ZENG S, BLANCHARD J, BREYSSE, SHI Y H, SU X T, NIE H, LID D. Mesoporous materials from zeolite seeds as supports for nickel- tungsten sulfide active phases[ J]. Appl Catal A, 2006, 298(1 ) : 88-93.
  • 9DING L H, ZHENG Y, ZHANG Z S, RING Z, CHEN J W. HDS, HDN, HAD and hydrocracking of model compounds over Mo-Ni catalysts with various acidities[J]. Appl Catal A, 2007, 319(1) : 25-37.
  • 10TOPSOE H. The role of Co-Mo-S type structures in hydrotreating catalysts[ J]. Appl Catal A 2007 322( 1 ) : 3-8.

二级参考文献22

  • 1李大东.炼油催化发展趋势[J].石油炼制与化工,1994,25(1):7-14. 被引量:8
  • 2靳广洲,樊秀菊,孙桂大,高俊斌,朱建华.碳化钼的制备与表征[J].无机材料学报,2007,22(3):504-508. 被引量:19
  • 3LECLERC Q L, PROVOST M, PASTOR H,LECLERCQ G. Catalytic properties of transition metal carbides[J]. J Catal, 1989,117(2) : 384-395.
  • 4OYAMA S T. Crystal structure and chemical reactivity of transition metal carbides and nitrides[J]. J Solid State Chem, 1992,96(2) : 442-445.
  • 5DOLCE G M, SAVAGE P E, THOMPSON L T. Hydrotreatment activities of supported molybdenum nitrides and carbides [ J]. Energy Fuels, 1997, 11(3) : 668-675.
  • 6LEDOUX M J, GALLOP D,YORK A P E. Molybdenum oxycarbide isomerization catalysts for cleaner fuel production[ J]. Catal Today, 1996, 27 (1-2) : 145-150.
  • 7LEVY R B, BOUDART M. Platinum-like behavior of tungsten carbide in surface catalysis[ J]. Science, 1973, 181(4099) : 547-549.
  • 8BRUNGS A J, YORK A P E, CLARIDGE J B, CARLOS M, GREEN M L H. Dry reforming of methane to synthesis gas over supported molybdenum carbide catalysts [ J ]. Catal Lett, 2000, 70 ( 3-4 ) : 117-122.
  • 9PATTERSON P, DAS T K, DAVIS B H, Carbon monoxide hydrogenation over molybdenum arid tungsten carbides[J]. Appl Catal A, 2003,251(2) : 449-455.
  • 10BOUCHY C, SCHMIDT I, ANDERSON J R, JACOBSEN C J H, DEROUANE E G, DEROUANE-ABD S B. Metastable fcc α-MoC1 -x supported on HZSM5 : Preparation and catalytic performance for the non-oxidative conversion of methane to aromatic compounds[ J ]. J Mol Catal A, 2000, 163(1-2) : 283-296.

共引文献80

同被引文献21

  • 1刘璞生,张忠东,高雄厚.稀土含量对Y型分子筛催化性能的影响[J].石油学报(石油加工),2010,26(S1):107-111. 被引量:12
  • 2李斌,李士杰,李能,刘从华,高雄厚,庞新梅.FCC催化剂中REHY分子筛的结构与酸性[J].催化学报,2005,26(4):301-306. 被引量:41
  • 3申建华,毛学文.焙烧气氛对REY沸石分子筛结构稳定性的影响[J].石油化工,1996,25(5):325-329. 被引量:9
  • 4何鸣元.催化裂化催化剂中Y型分子筛制造的水热化学[J].大自然探索,1996,15(4):12-13. 被引量:15
  • 5TONETI'O G, ATIAS J, DE LASA H. FCC catalysts with different zeolite crystallite sizes: acidity, structural properties and reactivity [ J ]. Applied Catalysis A : General, 2004, 270 (1-2) : 9-25.
  • 6YONG K P, LEE C W, KANG N Y, et al. Catalytic cracking of lower-valued hydrocarbons for producing light olefins[ J]. 2010, 14(2) : 75-84.
  • 7AL-KHATI'AF S. The influence of Y-zeolite unit cell size on the performance of FCC catalysts during gas oil catalytic cracking[ J ]. Applied Catalysis A : General,2002,231 (1-2) :293-306.
  • 8FLOCKHART B D, LIEW K Y, PINK R C. Alkylation of toluene with propene using zeolite catalysts [ J ]. Journal of Ca- talysis, 1981, 72(2) : 314-321.
  • 9XIAO S Y , LE VAN MAO R, DENES G. Methods for preparing thermally stable and active acid catalysts by incorporation of lanthanum into Y, desilicated Y and X zeolites[J]. Journal of Materials Chemistry, 1995, 5(8) : 1251-1255.
  • 10ZHAO Z K, QIAO W H, WANG G W, et al. Alkylation of α-methylnaphthalene with long-chain olefins catalyzed by rare earth lanthanum modified HY zeolite [ J ]. Journal of Molecular Catalysis A: Chemical, 2006, 250 (1-2) : 50-56.

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