物理化学学报 >> 2009, Vol. 25 >> Issue (08): 1517-1522.doi: 10.3866/PKU.WHXB20090723

研究论文 上一篇    下一篇

Ni/MgO-Al2O3催化剂上高温焦油组分的催化转化

艾馨鹏, 岳宝华, 汪学广, 杨军, 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|上海大学理学院化学系, 上海 200444
  • 收稿日期:2009-02-08 修回日期:2009-04-03 发布日期:2009-07-16
  • 通讯作者: 汪学广, 丁伟中 E-mail:wxg228@shu.edu.cn; wzding@shu.edu.cn

Catalytic Conversion of Tar Components in Hot Coke Oven Gas over Ni/MgO-Al2O3 Catalysts

AI Xin-Peng, YUE Bao-Hua, WANG Xue-Guang, YANG Jun, LU Xiong-Gang, DING Wei-Zhong   

  1. Shanghai Key Laboratory of Modern Metallurgy and Material Processing, Shanghai University, Shanghai 200072, P. R. China|Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, P. R. China
  • Received:2009-02-08 Revised:2009-04-03 Published:2009-07-16
  • Contact: WANG Xue-Guang, DING Wei-Zhong E-mail:wxg228@shu.edu.cn; wzding@shu.edu.cn

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摘要：

采用分步浸渍法制备了MgO-Al2O3负载的Ni基催化剂, 并运用N2吸附、载射线衍射(XRD)、透射电子显微镜(TEM)等手段进行表征. 该催化剂用于甲苯或萘为焦油模拟化合物的高温焦炉煤气(COG)的常压加氢裂解反应, 并考察了H2浓度、H2S对催化剂活性的影响. 结果表明: 催化剂还原后, 表面形成均匀分散、直径为8-14 nm的金属Ni纳米颗粒; 在较低的水碳摩尔比(nH2O/nC=0.28)时, 甲苯就能完全转化并选择性地加氢裂解形成CH4, 测试的时间内(480 min), 催化剂没有明显的失活和积炭现象, 显示出好的反应活性、稳定性和耐硫能力. 制得的Ni/MgO-Al2O3催化剂有望应用于较低水含量(10%-15%(φ, 体积分数))的高温焦炉煤气中焦油的直接转化.

关键词: 焦油, 焦炉煤气, 甲苯, 镍催化剂, 加氢裂化

Abstract:

NiO/MgO-Al2O3 catalysts with different Ni contents were prepared by a two-step impregnation method and characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) and transmission electron microscopy (TEM). Results showed that metallic Ni nanoparticles with diameters of 8-14 nm were formed and homogenously dispersed on the surface of the catalysts after reduction at 800 ℃. The catalysts were used for the catalytic conversion of toluene as a model tar compound in hot coke oven gas (COG) and showed excellent catalytic activity, stability and sulfur tolerance. Toluene could be fully converted and selectively hydrogenated to CH4 even using a low molar ratio of water to carbon (nH2O/nC=0.28) at 800 ℃ and under ambient pressure. The existence of H2O in the feed gas greatly enhanced the conversion of toluene and contributed to CH4 formation. Under similar conditions, naphthalene was converted into light fuel gases. Effects of H2 concentration and H2S in the feed gas were discussed. The Ni/MgO-Al2O3 catalyst was promising for the hydrocracking of tar compounds in hot coke oven gas with a low H2O content of 10%-15% (φ, volume fraction).

Key words: Tar, Coke oven gas, Toluene, Ni catalyst, Hydrocracking