镁铝混合氧化物负载镍催化剂上液化石油气的预重整

doi:10.3724/SP.J.1088.2012.20138

催化学报 ›› 2012, Vol. 33 ›› Issue (7): 1176-1182.DOI: 10.3724/SP.J.1088.2012.20138

镁铝混合氧化物负载镍催化剂上液化石油气的预重整

王新星, 汪学广*, 尚兴付, 聂望欣, 邹秀晶, 鲁雄钢, 丁伟中

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:2012-01-16 修回日期:2012-02-24 出版日期:2012-06-21 发布日期:2012-06-21

Pre-reforming of Liquefied Petroleum Gas over Magnesium Aluminum Mixed Oxide Supported Nickel Catalysts

WANG Xinxing, WANG Xueguang*, SHANG Xingfu, NIE Wangxin, ZOU Xiujing, LU Xionggang, DING Weizhong

Shanghai Key Laboratory of Modern Metallurgy and Material Processing, Shanghai University, Shanghai 200072, China

Received:2012-01-16 Revised:2012-02-24 Online:2012-06-21 Published:2012-06-21

摘要/Abstract

摘要： 采用共沉淀-浸渍法并在较低温度 (400~700 ^oC) 下焙烧制备了镁铝混合氧化物 (MgmAl) 负载的 Ni 催化剂. X 射线衍射和程序升温还原结果表明, Ni 物种高度分散于催化剂表面, 没有形成尖晶石 NiAl₂O₄. 在 650 ^oC 可被还原成金属 Ni 纳米晶粒, 在 400 ^oC 和较低水/碳摩尔比 (S/C = 2) 条件下表现出较好的催化液化石油气 (LPG) 重整反应性能. 详细考察了 Mg/Al 摩尔比、Ni 负载量、载体和催化剂的焙烧温度对催化剂活性和稳定性的影响. 结果表明, 由 500 ^oC 焙烧的 Mg_1.25Al 载体负载的 15%Ni 催化剂, 并于 500 ^oC 焙烧时, 在 LPG 重整反应中表现出最优的性能, 尽管它比高温 (≥ 800 ^oC) 焙烧制备的 Ni/MgmAl 催化剂更易积炭, 催化活性和稳定性有所下降, 但由于还原温度较低, 在交通和小规模供电的燃料电池领域更具实际应用意义.

关键词: 镍催化剂, 镁铝混合氧化物, 液化石油气, 预重整, 水蒸气重整

Abstract: The catalytic performance of Ni catalysts supported on magnesium aluminum mixed oxide (Ni/Mg_mAl) for the pre-reforming of liquefied petroleum gas (LPG) was studied, and the catalysts were prepared by the co-precipitation-impregnation method and calcined in the lower temperature range of 400–700 ^oC. The X-ray diffraction and H₂temperature-programmed reduction results showed that Ni species were highly dispersed on the catalyst surface without NiAl₂O₄ spinel formation. The Ni/Mg_mAl catalysts could be reduced to metallic Ni nanoparticles at 650 ^oC, which showed excellent catalytic activity and stability for LPG pre-reforming at 400 ^oC and a low steam/carbon molar ratio of 2.0. The effects of Mg/Al molar ratios, Ni loading, and calcination temperature of the support and catalyst on the catalytic behavior of the Ni/Mg_mAl catalysts were investigated in detail. The results revealed that the 15%Ni/Mg_1.25Al catalyst with both support and catalyst calcined at 500 ^oC had the optimal catalytic performance for LPG pre-reforming. Compared with Ni/Mg_mAl catalysts calcined at high temperature (≥ 800 ^oC), the present catalysts showed easier coke deposition and a slight decrease in catalytic activity and stability. However, it may be more promising candidate for LPG pre-reforming for the use of hydrogen fuel cells in transportation and small stationary application due to lower reduction temperature.

Key words: nickel catalyst, magnesium aluminum mixed oxide, liquefied petroleum gas, pre-reforming, steam reforming

王新星, 汪学广, 尚兴付, 聂望欣, 邹秀晶, 鲁雄钢, 丁伟中. 镁铝混合氧化物负载镍催化剂上液化石油气的预重整[J]. 催化学报, 2012, 33(7): 1176-1182.

WANG Xin-Xing, WANG Xue-Guang, SHANG Xing-Fu, NIE Wang-Xin, ZOU Xiu-Jing, LU Xiong-Gang, DING Wei-Zhong. Pre-reforming of Liquefied Petroleum Gas over Magnesium Aluminum Mixed Oxide Supported Nickel Catalysts[J]. Chinese Journal of Catalysis, 2012, 33(7): 1176-1182.

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镁铝混合氧化物负载镍催化剂上液化石油气的预重整

Pre-reforming of Liquefied Petroleum Gas over Magnesium Aluminum Mixed Oxide Supported Nickel Catalysts

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