欢迎登录材料期刊网

材料期刊网

高级检索

研究了柴油机NOx存储还原技术(NSR)浓燃再生阶段中NO还原反应.发展了铂催化剂表面H2还原NO的详细化学反应机理,包括6种气相组分、10种表面组分及28步基元反应,其中包含了主要含氮产物N2及副产物N2O和NH3的生成路径.此机理与CHEMKIN软件中的活塞流反应器(PFR)模型耦合进行数值模拟,反应器出口各组分体积分数预测结果与文献中实验数据吻合良好.在NO体积分数为500×10-6、反应器入口温度为270℃的条件下分析了进气中H2体积分数((100~2500)×10-6)对含氮产物选择性的影响.结果表明,H2体积分数小于500×10-6时,N2和N2O为主要的含氮产物;随着H2体积分数逐渐升高,当ψ(NO)/ψ(H2)高于1.5时,NH3成为主要产物.由敏感性分析结果可知,NH3对H2吸附反应的敏感性系数最大,提高该反应速率将促进NH3的生成.

参考文献

[1] Pio Forzatti;Luca Lietti;Isabella Nova .Diesel NO_x aftertreatment catalytic technologies: Analogies in LNT and SCR catalytic chemistry[J].Catalysis Today,2010(3/4):202-211.
[2] 苏庆运,王胜,李艳宾,帅石金,王建昕.柴油机LNT浓燃过程中铑表面CO还原NO的详细反应机理[J].汽车安全与节能学报,2012(01):51-57.
[3] Yi Liu;Yang Zheng;Michael P. Harold.Lean NO_x reduction on LNT-SCR dual-layer catalysts by H2 and CO[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2013:293-303.
[4] Dhainaut F;Pietrzyk S;Granger P .Kinetics of the NO/H-2 reaction on Pt/LaCoO3: A combined theoretical and experimental study[J].Journal of Catalysis,2008(2):296-305.
[5] Jin Wang;Yaying Ji;Vencon Easterling .The effect of regeneration conditions on the selectivity of NO_x reduction in a fully formulated lean NO_x trap catalyst[J].Catalysis Today,2011(1):83-92.
[6] Xu J;Clayton R;Balakotaiah V;Harold MP .Experimental and microkinetic modeling of steady-state NO reduction by H-2 on Pt/BaO/Al2O3 monolith catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):395-408.
[7] Qingyun Su;Yanbin Li;Sheng Wang .Detailed Mechanism for Reduction of N2O over Rhodium by CO in Automotive Exhaust[J].Topics in Catalysis,2013(1/8):345-351.
[8] 苏庆运,马兵,陈家骅,李艳宾,徐康.柴油机LNT再生过程中铑表面H2还原NOx的详细反应机理[J].内燃机学报,2013(04):349-353.
[9] J. Koop;O. Deutschmann .Detailed surface reaction mechanism for Pt-catalyzed abatement of automotive exhaust gases[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2009(1/2):47-58.
[10] Kondratenko VA;Baerns M .Mechanistic insights into the formation of N2O and N-2 in NO reduction by NH3 over a polycrystalline platinum catalyst[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(26):111-118.
[11] Sadhankar RR.;Lynch DT. .SLOW CONVERGENCE TO CYCLE-INVARIANCE DURING FORCED OSCILLATIONS OF THE NO+CO REACTION OVER A PT CATALYST[J].Chemical Engineering Science,1996(10):2061-2068.
[12] R.Burch;S.T.Daniells;J.P.Breen;P.Hu .A combined transient and computational study of the dissociation of N_2O on platinum catalysts[J].Journal of Catalysis,2004(2):252-260.
[13] Daniel Chatterjee;Olaf Deutschmann;Jurgen Warnatz .Detailed surface reaction mechanism in a three-way catalyst[J].Faraday discussions,2001(119):371-384.
[14] Gerard Novell-Leruth;Ana Valcarcel;Javier Pérez-Ramírez;Josep M. Ricart .Ammonia Dehydrogenation over Platinum-Group Metal Surfaces. Structure, Stability, and Reactivity of Adsorbed NHx Species[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(2):860-868.
[15] Prasanna R. Dasari;Rachel Muncrief;Michael P. Harold .Elucidating NH3 formation during NO_x reduction by CO on Pt-BaO/Al2O3 in excess water[J].Catalysis Today,2012(1):43-53.
[16] Jin Xu;Michael P. Harold;Vemuri Balakotaiah .Microkinetic modeling of steady-state NO/H2/O2 on Pt/BaO/Al2O3 NO_x storage and reduction monolith catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2009(1/2):73-86.
[17] Denise C. Ford;Ye Xu;Manos Mavrikakis .Atomic and molecular adsorption on Pt(111)[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2005(3):159-174.
上一张 下一张
上一张 下一张
计量
  • 下载量()
  • 访问量()
文章评分
  • 您的评分:
  • 1
    0%
  • 2
    0%
  • 3
    0%
  • 4
    0%
  • 5
    0%