自蔓延燃烧法制备Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy催化剂催化NO制NH3反应的性能研究

闫瑞宁,王一男,赵旭腾,刘旻,刘兴,胡琨,石福禄,王涛,林赫,黄震

车用发动机 ›› 2021, Vol. 0 ›› Issue (3) : 50-57.

车用发动机 ›› 2021, Vol. 0 ›› Issue (3) : 50-57. DOI: 10.3969/j.issn.1001-2222.2021.03.009
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自蔓延燃烧法制备Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy催化剂催化NO制NH3反应的性能研究

  • 闫瑞宁1,王一男1,赵旭腾1,刘旻1,刘兴2,胡琨2,石福禄3,王涛3,林赫1,黄震1
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Catalytic Performance for the Reaction from NO to Ammonia of Pd 0.01CuxCe(1-x)/2Zr(1-x)/2Oy Prepared by Self-Propagating High Temperature Synthesis

  • YAN Ruining1,WANG Yi'nan1,ZHAO Xuteng1,LIU Min1,LIU Xing2,HU Kun2,SHI Fulu3,WANG Tao3,LIN He1,HUANG Zhen1
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摘要

被动式氨SCR系统是一种应用在稀燃发动机,可减少NOx排放,生产SCR用氨的后处理方法,该系统使用NO与H2作为原料气在催化剂的作用下产生氨气用于后续SCR脱硝。通过试验研究,采用自蔓延燃烧合成(SHS)法合成了Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy(x=0,0.1,0.2,0.4)催化剂。用XRD、BET、Raman、H2-TPR、XPS、原位表征等方法研究了它们的催化活性。建立了Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy(x=0,0.1,0.2,0.4)催化剂的反应性与物种组成、酸性质和氧化还原性能的关系。结果表明,适量的铜掺杂可以形成更多的酸性位点,调节表面元素的价态分布,有助于产生更高的催化效率。其中,Pd0.01Cu0.1Ce0.45Zr0.45Ox的氨转化率最高,反应温度窗口较宽(225~375 ℃),NO向NH3转化率大于90%。这是由于高度分散的CuO增强了CuO与Ce0.5Zr0.5O2载体之间的相互作用,从而提高了催化活性。

Abstract

The passive ammonia SCR system is a novel aftertreatment method for lean-burn engine to reduce NOx emission and produce necessary ammonia for SCR. The reaction between NO and H2 was activated and ammonia gas of SCR, denitration was then prepared under the action of a catalyst. Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy catalysts with x parameter of 0, 0.1, 0.2 and 0.4 were synthesized through self-propagating combustion reaction method. The activities of catalysts were investigated according to XRD, BET, Raman, H2-TPR, XPS, in situ DRIFTS. The relationship between the catalyst reactivity and species composition, acid property, and redox behavior was established in the end. The results showed that a moderate amount of Cu doping could significantly form more acid sites and tune the valence distribution of surface elements so as to lead to a high catalytic efficiency. Pd0.01Cu0.1Ce0.45Zr0.45Ox had the highest ammonia conversion rate among all the catalysts with a wide reaction temperature window of 225-375 ℃. The conversion rate of NO to NH3 was beyond 90% with the catalyst due to the improved catalytic activity led by the fact that highly-dispersed CuO enhanced the interaction between CuO and Ce0.5Zr0.5O2 carrier.

关键词

选择性催化还原 / 催化剂 / 制备 / 自蔓延燃烧合成法

Key words

SCR / catalyst / preparation / self-propagating high temperature synthesis

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闫瑞宁,王一男,赵旭腾,刘旻,刘兴,胡琨,石福禄,王涛,林赫,黄震. 自蔓延燃烧法制备Pd0.01CuxCe(1-x)/2Zr(1-x)/2Oy催化剂催化NO制NH3反应的性能研究[J]. 车用发动机. 2021, 0(3): 50-57 https://doi.org/10.3969/j.issn.1001-2222.2021.03.009
YAN Ruining,WANG Yi'nan,ZHAO Xuteng,LIU Min,LIU Xing,HU Kun,SHI Fulu,WANG Tao,LIN He,HUANG Zhen. Catalytic Performance for the Reaction from NO to Ammonia of Pd 0.01CuxCe(1-x)/2Zr(1-x)/2Oy Prepared by Self-Propagating High Temperature Synthesis[J]. Vehicle Engine. 2021, 0(3): 50-57 https://doi.org/10.3969/j.issn.1001-2222.2021.03.009

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