PDF(1386 KB)
Preparation of monolithic catalysts and their performance in the hydrodesulfurization of thiophene
XING Jun;ZHU JiQin*;LI JianWei;LIU Hui;LI ChengYue
Journal of Beijing University of Chemical Technology ›› 2009, Vol. 36 ›› Issue (6) : 27-32.
PDF(1386 KB)
PDF(1386 KB)
Preparation of monolithic catalysts and their performance in the hydrodesulfurization of thiophene
Cordierite monolithic catalysts were prepared by loading the industrial hydrodesulfurization catalyst FHUDS. The structure of the catalysts was characterized by means of XRD, N-2 adsorption/desorption measurements, SEM and XPS. Theircatalytic performance in hydrodesulfurization (HDS) was evaluated in a fixed bed reactor by taking thiophene hydrodesulfurization as a model reaction. The results indicated that the surface area of cordierite was increased and Al3+and Mg2+ ions were removed from the silicate structure by acid pretreatment, but the crystal structure of the cordierite was unchanged. The performance of the monolithic catalysts was influenced by the pretreatment conditions of the cordierite, the coating pH value and the hole extender. Under conditions giving cordierite with the required mechanical properties, increasing concentrations of acid and longer boiling times led to better catalyst coating properties and catalytic performance in hydrodesulfurization. It was found that the monolithic catalysts loaded with the active colloid at pH 3, prepared with cordierite boiled for 4?h with 50% oxalic acid exhibited the highest HDS activity, with the conversion of thiophene reaching 95% at 350?℃. The catalyst performance was enhanced by theaddition of appropriate amounts of urea to the colloid, with the conversion of thiophene increasing from 66% to 77% at 300?℃, and from 78% to 91% at 325℃.
［1］朱全力, 章秋霖, 柯东贤, 等. 负载型碳氧化钼催化剂的制备及其二苯并噻吩的HDS活性［J］. 燃料化学学报, 2008, 36(3): 316-321.
Zhu Q L, Zhang Q L, Ke D X, et al. Preparation of γAl2O3supported molybdenum oxycarbide catalyst and its HDS activity［J］. Journal of Fuel Chemistry and Technology, 2008, 36(3): 316-321. (in Chinese)
［2］温钦武, 沈健, 韩英, 等. 柴油加氢脱硫催化剂的研究进展［J］. 炼油技术与工程, 2007, 37(3): 48-51.
Wen Q W, Shen J, Han Y, et al. Research and development of diesel oil hydrodesulfurization catalyst［J］. Petroleum Refinery Engineering, 2007, 37(3): 48-51. (in Chinese)
［3］PérezCadenas A F, Kapteijn F, Moulijn J A, et al. Pd and Pt catalysts supported on carboncoated monoliths for lowtemperature combustion of xylenes［J］. Catalysis Today, 2006, 44(12): 2463-2468.
［4］MaldonadoHódar F J, MorenoCastilla C, PérezCadenas A F. Catalytic combustion of toluene on platinumcontaining monolithic carbon aerogels［J］. Applied Catalysis B: Environmental, 2004, 54(4): 217-224.
［5］华金铭, 郑起, 林性怡, 等. 整体式高温水煤气变换催化剂的初步研制［J］. 工业催化, 2003, 11(3): 16-20.
Hua J M, Zhen Q, Lin X Y, et al. Development of monolithic catalysts for hightemperature watergas shift reaction［J］. Industrial Catalysis, 2003, 11(3): 16-20. (in Chinese)
［6］PérezCadenas A F, Zieverink M M P, Kapteijn F, et al. High performance monolithic catalysts [JP2]for hydrogenation reactions［J］. Catalysis Today, 2005, 105(2): 623-[JP]628.
［7］Meille V. Review on methods to deposit catalysts on structured surfaces［J］. Applied Catalysis A: General, 2006, 315: 1-17.
［8］Nijhuis T A, Kreutzer M T, Romijn A C J, et al. Monolithic catalysts as efficient threephase reactors［J］. Chemical Engineering Science, 2001, 56(3): 823-829.［9］史志铭, 梁开明, 顾守仁, 等. 元素掺杂对堇青石晶体结构及热膨胀系数的作用［J］. 现代技术陶瓷, 2000(2): 18-23.
Shi Z M, Liang K M, Gu S R, et al. Effects of elementsdoping on the crystal structure and thermal expansion coefficient of cordierite［J］. Advanced Ceramics, 2000(2): 18-23. (in Chinese)
［10］Shigapov A N, Graham G W, McCabe R W, et al. The preparation of highsurfacearea cordierite monolith by acid treatment［J］. Applied Catalysis A: General, 1999, 182(1): 137-146.
［11］Elmer T H. Selective leaching of extruded cordierite honeycomb structures［J］. Ceramic Engineering and Science Proceedings, 1986, 7(1/2): 40-51.
［12］孙杰兵, 熊锐, 王世敏, 等. 三氧化钼薄膜的制备和结构研究［J］. 武汉大学学报: 理学版, 2002, 48(5): 589-592.
Sun J B, Xiong R, Wang S M, et al. Preparation and structure study molybdenum oxide thin films by solgel process［J］. Wuhan University Journal: Natural Science Edition, 2002, 48(5): 589-592. (in Chinese)
［13］Sotiropoulou D, Yiokari C, Vayenas C G, et al. An Xray photoelectron spectroscopy study of zirconiasupported Mo and NiMo hydrodesulfurization catalysts［J］. Applied Catalysis A: General, 1999, 183(1): 15-22.
［14］Li D, Sato T, Imamura M, et al. Spectroscopic characterization of NiMo/γAl2O3B2O3 catalysts for hydrodesulfurization of dibenzothiophene［J］. Journal of Catalysis, 1997, 170(1): 357-365.
［15］付会娟, 金月昶, 康久常. 蜂窝陶瓷载体上氧化铝涂层的制备［J］. 当代化工, 2006, 35(5): 289-296.
Fu H J, Jin Y C, Kang J C. Preparation of Al2O3 washcoat deposited on ceramic honeycombs［J］. Contemporary Chemical Industry, 2006, 35(5): 289-296. (in Chinese)
PDF(1386 KB)
/
| 〈 |
|
〉 |
