Ni基催化剂催化燃油重整耦合选择性催化还原NOx反应

doi:10.1016/S1872-2067(12)60598-1

催化学报

Ni基催化剂催化燃油重整耦合选择性催化还原NO_x反应

赵娇娇, 余运波, 韩雪, 贺泓

中国科学院生态环境研究中心, 北京 100085

收稿日期:2013-02-07 修回日期:2013-04-02 出版日期:2013-07-16 发布日期:2013-07-16
通讯作者: 余运波
基金资助:
国家自然科学基金(21177142); 国家重点基础研究发展计划(973计划, 2010CB732304); 国家高技术研究发展计划(863计划, 2013AA065301).

Fuel reforming over Ni-based catalysts coupled with selective catalytic reduction of NO_x

ZHAO Jiaojiao, YU Yunbo, HAN Xue, HE Hong

Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China

Received:2013-02-07 Revised:2013-04-02 Online:2013-07-16 Published:2013-07-16
Supported by:
This work was supported by the National Natural Science Foundation of China (21177142), the National Basic Research Program of China (973 Program, 2010CB732304), and the National High Technology Research and Development Program of China (863 Program, 2013AA065301).

摘要/Abstract

摘要： 分别以La₂O₂CO₃, CeO₂, ZrO₂和Al₂O₃为载体, 采用浸渍法制备了Ni基重整催化剂, 并以正十二烷模拟车载燃油进行催化重整反应以同时制备小分子碳氢化合物(HCs)和H₂, 考察了其在4wt%Ag/Al₂O₃上选择性催化还原(HC-SCR)氮氧化物(NO_x)的性能. 采用N₂吸附-脱附、X射线粉末衍射、H₂程序升温还原和热重等手段对Ni基催化剂进行了表征. 结果表明, 随着重整催化剂氧化还原性能增强, 产物中H₂浓度增加, 可参与SCR反应的HCs含量减少, 从而导致重整-SCR耦合体系上NO_x净化活性温度窗口向低温移动, NO_x最高转化率降低. Ni/ZrO₂+Ag/Al₂O₃耦合体系中H₂/HCs符合SCR反应所需的最优比例, 在柴油车典型排气温度范围内表现出良好的NO_x净化能力. 同时, 在Ni/ZrO₂+Ag/Al₂O₃耦合体系上考察了其燃油重整-SCR的活性稳定性. 结果显示, 重整催化剂的耐久性有待进一步提高.

关键词: 燃油重整, 镍基催化剂, 氮氧化物, 选择性催化还原, 银, 氧化铝

Abstract: La₂O₂CO₃, CeO₂, ZrO₂, and Al₂O₃ supported Ni catalysts were prepared by an impregnation method and employed for reforming of n-dodecane to simultaneously produce low molecular weight hydrocarbons (HCs) and H₂. These reforming products served as reductants and promoters for the selective catalytic reduction (SCR) of NO_x over Ag/Al₂O₃. N₂ adsorption-desorption, X-Ray powder diffraction, H₂ temperature programmed reduction, and thermogravimetric analysis were performed for Ni-based catalysts. It was shown that an increase in the redox performance of Ni-based catalysts enhanced the H₂ production from fuel reforming but decreased the amount of HCs available for further SCR reaction. The temperature window for NO_x removal using the coupled system shifted to lower temperatures at the expense of the NO_x conversion. An optimal ratio of H₂/HCs was achieved using a Ni/ZrO₂+Ag/Al₂O₃dual catalyst system, which exhibited high activity for NO_x conversion at typical diesel exhaust temperatures. Studies on the durability and performance of this Ni/ZrO₂+Ag/Al₂O₃coupled system were also performed, and the results showed that the lifetime of the reforming catalyst may limit the system and requires further improvement.

Key words: Catalytic reforming, Ni-based catalyst, Nitrogen oxide, Selective catalytic reduction, Silver, Alumina

赵娇娇, 余运波, 韩雪, 贺泓. Ni基催化剂催化燃油重整耦合选择性催化还原NO_x反应[J]. 催化学报, DOI: 10.1016/S1872-2067(12)60598-1.

ZHAO Jiaojiao, YU Yunbo, HAN Xue, HE Hong. Fuel reforming over Ni-based catalysts coupled with selective catalytic reduction of NO_x[J]. Chinese Journal of Catalysis, DOI: 10.1016/S1872-2067(12)60598-1.

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Ni基催化剂催化燃油重整耦合选择性催化还原NO_x反应

Fuel reforming over Ni-based catalysts coupled with selective catalytic reduction of NO_x

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Ni基催化剂催化燃油重整耦合选择性催化还原NOx反应

Fuel reforming over Ni-based catalysts coupled with selective catalytic reduction of NOx

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Ni基催化剂催化燃油重整耦合选择性催化还原NO_x反应

Fuel reforming over Ni-based catalysts coupled with selective catalytic reduction of NO_x