催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (3): 456-462.DOI: 10.3724/SP.J.1088.2011.01034

• 研究论文 • 上一篇    下一篇

低水碳比条件下 Ni/CeO2/Al2O3 催化剂上液化石油气的预重整

赵景月, 邹秀晶, 汪学广, 刘合之, 李林, 鲁雄刚, 丁伟中   

  1. 上海大学上海市现代冶金与材料制备重点实验室, 上海 200072
  • 收稿日期:2010-10-20 修回日期:2010-11-12 出版日期:2011-03-04 发布日期:2014-08-01

Pre-reforming of Liquefied Petroleum Gas over Ni/CeO2/Al2O3 Catalyst under Low Molar Ratios of Steam to Carbon

ZHAO Jingyue, ZOU Xiujing, WANG Xueguang*, LIU Hezhi, LI Lin, LU Xionggang, DING Weizhong*   

  1. Shanghai Key Laboratory of Modern Metallurgy and Material Processing, Shanghai University, Shanghai 200072, China
  • Received:2010-10-20 Revised:2010-11-12 Online:2011-03-04 Published:2014-08-01

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摘要： 采用硝酸盐溶液共浸渍薄水铝石制备了不同 Ni 含量的 Ni/CeO2/Al2O3 催化剂, 并采用 X 射线衍射、N2 物理吸附和程序升温还原等手段对其进行了表征. 结果表明, Ni 和 CeO2 物种之间存在较强的相互作用, CeO2 的加入有利于 NiAl2O4 还原成金属 Ni, 而金属 Ni 又促进了 CeO2 还原并与 Al2O3 反应形成 CeAlO3. 详细研究了 Ni/CeO2/Al2O3 催化剂在低水碳摩尔比条件下催化预重整液化石油气 (LPG) 的反应性能, 考察了 Ni 含量、反应温度和水碳摩尔比对催化剂性能的影响. 结果表明, 在 275 ~ 375 oC 的条件下, 催化剂表现出很高的 LPG 预重整反应活性. 较高的 Ni 含量和水碳摩尔比不仅有利于 LPG 重整为 H2 和碳氧化物, 也有利于碳氧化物和 H2 的甲烷化反应. Ni/CeO2/Al2O3 催化剂在低水碳摩尔比条件下表现出较高的稳定性和优良的抗积炭性能. 提出了在低水碳摩尔比条件下高碳烷烃预重整的反应机理.

关键词: 镍, 氧化铈, 氧化铝, 液化石油气, 预重整, 水碳比

Abstract: Ni/CeO2/Al2O3 catalyst samples with different Ni contents were prepared by co-impregnating boehmite with aqueous solution of cerium and nickel nitrates and characterized by X-ray diffraction, N2 adsorption, and temperature-programmed reduction. It was found that there was a strong interaction between Ni and CeO2 species. Addition of CeO2 promoted the reduction of NiAl2O4 to metal Ni, while nickel species in turn promoted the reduction of CeO2 and reacted with Al2O3 to CeAlO3. The pre-reforming of commercial liquefied petroleum gas (LPG) was investigated over Ni/CeO2/Al2O3 catalyst at low steam/carbon molar ratios (less than 1.0). The effects of Ni content, reaction temperature, and S/C molar ratio on the performance of the Ni/CeO2/Al2O3 catalyst were discussed. The results showed that the catalyst was highly active and stable for the steam reforming of LPG at 275–375 °C. Higher Ni content and S/C ratio promoted the steam reforming of LPG and substantially accelerated the methanation of COx and H2. The stability tests indicated that the Ni/CeO2/Al2O3 catalyst exhibited excellent stability and resistance to carbon deposition. The reaction mechanism for pre-reforming of higher hydrocarbons under lower S/C molar ratios was proposed.

Key words: nickel, ceria, alumina, liquefied petroleum gas, pre-reforming, steam/carbon molar ratio