欢迎登录材料期刊网

材料期刊网

高级检索

以硝酸亚铈(Ce(NO3)3·6H2O)和正硅酸四乙酯(C8H20O4Si)为前驱体,采用溶胶-凝胶法合成了系列具有大比表面积的xCeO2-(1-x)SiO2 (x=0,0.25,0.50,0.75,1)复合氧化物载体,然后浸渍活性组分Ni制得用于甲烷部分氧化制合成气的Ni催化剂.运用N2物理吸附-脱附、X射线粉末衍射、扫描电镜、紫外-可见漫反射光谱、氢程序升温还原、氨程序升温脱附和热重等手段对所得催化剂的组织结构、还原性、表面酸性和积炭行为等进行了表征;同时考察了催化剂的组成、焙烧温度和反应时间等对催化剂在甲烷部分氧化制合成气中催化性能的影响.表征结果表明,该系列Ni/CeO2-SiO2催化剂具有大比表面积,CeO2晶粒较小,NiO的分散性好且易被还原,表面酸性弱,不容易积炭.当Ce/Si摩尔比为1∶1,活性组分Ni的质量分数为10%,焙烧温度为700℃时,所制备的Ni/CeO2-SiO2催化剂表现出较好的稳定性、最高的CH4转化率(~84%)和对产物CO及H2的选择性(>87%).

参考文献

[1] Korup, O.;Goldsmith, C.F.;Weinberg, G.;Geske, M.;Kandemir, T.;Schl?gl, R.;Horn, R..Catalytic partial oxidation of methane on platinum investigated by spatial reactor profiles, spatially resolved spectroscopy, and microkinetic modeling[J].Journal of Catalysis,2013:1-16.
[2] 余长林,胡久彪,杨凯,周晓春.制备方法对Ni/CeO2-Al2O3催化剂甲烷部分氧化催化性能的影响[J].燃料化学学报,2013(06):722-728.
[3] 仙存妮,王少飞,孙春文,李泓,陈晓惠,陈立泉.Ni掺杂对纳米结构牡丹花状CeO2材料催化特性的影响[J].催化学报,2013(02):305-312.
[4] Sabori R;Sharifnia S;Aalami-Aleagha M E;Panahi M R .[J].Journal of the Taiwan Institute of Chemical Engineers,2012,43:153.
[5] Yu C L;Weng W Z;Shu Q;Meng X J Zhang B Chen X R Zhou X C .[J].Journal of Natural Gas Chemistry,2011,20:135.
[6] 刘瑞艳,杨美华,黄传敬,翁维正,万惠霖.介孔Co-Al2O3催化剂上甲烷部分氧化制合成气[J].催化学报,2013(01):146-151.
[7] Babakhani E G;Towfighi J;Taheri Z;Pour A N Zekordi M Taheri A .[J].Journal of Natural Gas Chemistry,2012,21:519.
[8] 杨民,Helmut PAPP.Pt/MgO 催化剂上甲烷部分氧化制合成气反应[J].催化学报,2008(03):228-232.
[9] Rodrigues L M T S;Silva R B;Rocha M G C;Bargiela P Noronha F B Brand(a)o S T .[J].Catalysis Today,2012,197:137.
[10] Mateos-Pedrero C;Duquesne S;Carrazáán S R G;Soria M A Ruíz P .[J].Applied Catalysis A: General,2011,394:245.
[11] Benrabaa R;Boukhlouf H;L(o)fberg A;Rubbens A Vannier R N Bordes-Richard E Barama A .[J].Journal of Natural Gas Chemistry,2012,21:595.
[12] 夏文生,常刚,侯玉慧,翁维正,万惠霖.Ni的化学态对甲烷部分氧化反应机理的影响:能学分析[J].物理化学学报,2011(07):1567-1573.
[13] Bayrakdar E;Altin(c)eki(c) T G;(O)ksüz(o)mer M A F .[J].FUEL PROCESSING TECHNOLOGY,2013,110:167.
[14] 余长林,周晓春,翁维正,胡久彪,陈喜蓉,魏龙福.碱土Sr对Co/Al2O3催化剂甲烷部分氧化反应的影响[J].燃料化学学报,2012(10):1222-1229.
[15] 温在恭,李虎,翁维正,夏文生,黄传敬,万惠霖.Rh/SiO2催化剂上甲烷部分氧化制合成气的反应机理[J].催化学报,2012(07):1183-1190.
[16] Zhu J Q;Peng X X;Yao L;Shen J Tong D M Hu C W .[J].International Journal of Hydrogen Energy,2011,36:7094.
[17] Salazar-Villalpando M D;Reyes B .[J].International Journal of Hydrogen Energy,2009,34:9723.
[18] Campa M C;Ferraris G;Gazzoli D;Pettiti I Pietrogiacomi D .[J].Applied Catalysis B: Environmental,2013,142-143:423.
[19] Maniecki T P;Bawolak K;Mierczy(n)ski P;Kaczorowski P Jó(z)wiak W K .[J].Kinetics and Catalysis,2011,52:711.
[20] 余长林,胡久彪,翁维正,周晓春,陈喜蓉.Co/Ce0.5Zr0.5O2催化剂的制备及甲烷部分氧化制合成气[J].燃料化学学报,2012(04):418-423.
[21] Larimi A S;Alavi S M .[J].FUEL,2012,102:366.
[22] Li B;Li H;WengW Z;Zhang Q Huang C J Wan H L .[J].FUEL,2013,103:1032.
[23] Xia W S;Hou Y H;Chang G;Weng W Z Han G B Wan H L .[J].International Journal of Hydrogen Energy,2012,37:8343.
[24] Li, L.;He, S.;Song, Y.;Zhao, J.;Ji, W.;Au, C.-T..Fine-tunable Ni@porous silica core-shell nanocatalysts: Synthesis, characterization, and catalytic properties in partial oxidation of methane to syngas[J].Journal of Catalysis,2012:54-64.
[25] Li B T;Xu X J;Zhang S Y .[J].International Journal of Hydrogen Energy,2013,38:890.
[26] Reddy B M;Khan A .[J].CATALYSIS SURVEYS FROM ASIA,2005,9:155.
[27] Reddy, BM;Reddy, GK;Ganesh, I;Ferreira, JMF .Single step synthesis of nanosized CeO2-M (x) O (y) mixed oxides (M (x) O (y) = SiO2, TiO2, ZrO2, and Al2O3) by microwave induced solution combustion synthesis: characterization and CO oxidation[J].Journal of Materials Science,2009(11):2743-2751.
[28] Li J S;Hao Y X;Li H J;Xia M Y Sun X Y Wang L J .[J].Microporous and Mesoporous Materials,2009,120:421.
[29] Roh H S;Eum I H;Jeong D W .[J].RENEWABLE ENERGY,2012,42:212.
[30] Kambolis A;Matralis H;Trovarelli A;Papadopoulou Ch .[J].Applied Catalysis A: General,2010,377:16.
[31] Rocchini E.;Vicario M.;Llorca J.;de Leitenburg C.;Dolcetti G. Trovarelli A. .Reduction and oxygen storage behavior of noble metals supported on silica-doped ceria[J].Journal of Catalysis,2002(2):407-421.
[32] Wang H Y;Bai Y L;Liu S;Wu J L Wong C P .[J].Acta Materialia,2002,50:4369.
[33] 叶平 .[D].上海:上海师范大学,2007.
[34] Lisboa J S;Terra L E;Silva P R J;Saitovitch H Passos F B .[J].FUEL PROCESSING TECHNOLOGY,2011,92:2075.
[35] Lisboa J d S;Santos D C R M;Passos F B;Noronha F B3 .[J].Catalysis Today,2005,101:15.
[36] Zapata B;Valenzuela M A;Palacios J;Torres-Garcia E .[J].International Journal of Hydrogen Energy,2010,35:12091.
[37] Chen J X;Wu Q Y;Zhang J X;Zhang J Y .[J].FUEL,2008,87:2901.
[38] Zeng S H;Wang L;Gong M C;Chen Y Q .[J].Journal of Natural Gas Chemistry,2010,19:509.
[39] (A)guila G;Gracia F;Araya P .[J].Applied Catalysis A: General,2008,343:16.
[40] Pino L;Vita A;Cipitì F;Laganà M Recupero V .[J].Applied Catalysis B: Environmental,2011,104:64.
[41] Silva F de A;RuizJ A C;de Souza K R;Bueno J M C Mattos L V Noronha F B Hori C E .[J].Applied Catalysis A: General,2009,364:122.
[42] Gao J;Guo J Z;Liang D;Hou Z Y Fei J H Zheng X M .[J].International Journal of Hydrogen Energy,2008,33:5493.
[43] Chen L;Lu Y;Hong Q;Lin J Dautzenberg F M .[J].Applied Catalysis A: General,2005,292:295.
[44] (O)zdemir H;(O)ksüz(o)mer M A F;Gürkaynak M A .[J].International Journal of Hydrogen Energy,2010,35:12147.
[45] SongY Q;Liu H M;Liu S Q;He D H .[J].Energy & Fuels,2009,23:1925.
[46] Choudhary T V;Choudhary V R .[J].Angewandte Chemie International Edition,2008,47:1828.
[47] Xu S;Zhao R;Wang X L .[J].FUEL PROCESSING TECHNOLOGY,2004,86:123.
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%