| Ni/MgO/Al2O3催化剂上以1-甲基萘为模型化合物高温焦炉煤气焦油的催化转化 |
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| 引用本文： | 杨军,汪学广,李林,沈葵,鲁雄刚,丁伟中. Ni/MgO/Al2O3催化剂上以1-甲基萘为模型化合物高温焦炉煤气焦油的催化转化[J]. 高等学校化学学报, 2010, 31(9): 1841 |
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| 作者姓名： | 杨军 汪学广 李林 沈葵 鲁雄刚 丁伟中 |
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| 作者单位： | 上海大学上海市现代冶金与材料制备重点实验室,上海,200072;上海大学上海市现代冶金与材料制备重点实验室,上海,200072;上海大学上海市现代冶金与材料制备重点实验室,上海,200072;上海大学上海市现代冶金与材料制备重点实验室,上海,200072;上海大学上海市现代冶金与材料制备重点实验室,上海,200072;上海大学上海市现代冶金与材料制备重点实验室,上海,200072 |
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| 基金项目： | 国家八六三计划项目,上海市科学技术委员会重点项目,上海市浦江人才计划,国家教育部留学回国人员科研启动资金资助项目 |
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| 摘 要： | 采用共浸渍薄水铝石(AlOOH)方法制备了一系列Ni/MgO/Al2O3催化剂, 并采用N2气吸附及Ｘ射线衍射等手段进行了表征. 选择1-甲基萘作为焦油模型化合物, 研究了该催化剂催化转化具有较低水蒸气/碳摩尔比(nH2O/nC) 的高温焦炉煤气(COG)中焦油催化反应性能. 考察了催化剂中MgO含量及反应条件等对催化剂性能的影响. 实验结果表明, 在775 ℃和nH2O/nC=0.7条件下, MgO改性的Ni/MgO/Al2O3催化剂对1-甲基萘催化转化为小分子气体反应具有较好的催化活性和稳定性; 热重分析表明, MgO的加入能显著提高催化剂的抗积炭能力. 在Ni/MgO/Al2O3催化剂上, 反应气中高浓度H2S气体(0.25%, 体积分数)能够促进焦油催化转化为小分子气体, 这可能是由于H2S在Ni表面的可逆吸附形成更适合于重整反应的活性位, 同时抑制了烷烃裂解吸附形成的碳在金属中的溶解、扩散并最终形成积炭过程.
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| 关 键 词： | 镍催化剂 1-甲基萘 焦炉煤气 焦油 催化转化 |
| 收稿时间： | 2010-01-21 |
Catalytic Conversion of 1-Methylnaphthalene as Tar Model Compound from Hot Coke Oven Gas over Ni/MgO/Al2O3 Catalysts |
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| YANG Jun,WANG Xue-Guang,LI Lin,SHEN Kui,LU Xiong-Gang,DING Wei-Zhong. Catalytic Conversion of 1-Methylnaphthalene as Tar Model Compound from Hot Coke Oven Gas over Ni/MgO/Al2O3 Catalysts[J]. Chemical Research In Chinese Universities, 2010, 31(9): 1841 |
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| Authors: | YANG Jun WANG Xue-Guang LI Lin SHEN Kui LU Xiong-Gang DING Wei-Zhong |
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| Affiliation: | Shanghai Key Laboratory of Modern Metallurgy and Material Processing, Shanghai University, Shanghai 200072, China |
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| Abstract: | A series of Ni/MgO/Al2O3 catalysts were prepared by the method of co-impregnating boehmite(AlOOH) and characterized using N2 adsorption and X-ray diffraction(XRD). 1-Methylnaphthalene was selected as a tar compound to investigate the performance of the Ni/MgO/Al2O3 catalysts for converting tar from hot coke oven gas(COG) with a low water to carbon molar ratio(nH2O/nC) into light fuel gases. The effects of MgO content and operating conditions were examined at 775 ℃ and nH2O/nC=0.7. The experimental results showed that the MgO modified Ni/MgO/Al2O3 catalysts possessed excellent catalytic activity and stability for the conversion of 1-methylnaphthalene to small gas molecules. TG analysis of the used catalysts showed that addition of MgO in the Ni/MgO/Al2O3 catalysts could significantly enhance resistance to carbon deposition. It was first found that the presence of higher concentration of H2S(0.25%, volume fraction) could promote the conversion of tar to small gas molecules over the Ni/MgO/Al2O3 catalysts. This might be because the reversible adsorption of H2S on the surface of metallic Ni led to the formation of ensemble of Ni sites more suitable for steam reforming and, meanwhile, inhibited dissolution and diffusion of carbon in metal Ni from dissociative adsorption of hydrocarbon, leading to the formation of coke disposition on the catalyst. |
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| Keywords: | Ni catalyst 1-Methylnaphthalene Coke oven gas Tar Catalytic conversion |
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