欢迎登录材料期刊网

材料期刊网

高级检索

采用10% H2S/H2对Ni2P/SiO2催化剂进行预处理,利用X射线衍射、电感耦合等离子发射光谱、X射线光电子能谱、CO化学吸附、H2程序升温脱附、NH3程序升温脱附及活性评价等方法研究了H2S预处理对催化剂结构和氯苯加氢脱氯反应性能的影响.结果表明,即使在873 K进行H2S预处理,Ni2P/SiO2催化剂体相结构及Ni2P晶粒大小没有发生变化,但导致Ni2P晶粒表面形成了磷硫镍相(NiPxSy),同时使表面溢流氢数量增加.硫物种的存在不仅阻塞了部分镍中心,使催化剂表面镍中心密度降低,也导致镍中心的缺电子性进一步增加.经H2S预处理后Ni2P/SiO2催化剂上氯苯加氢脱氯反应的转化频率(TOF)明显提高,这可能与催化剂表面Ni物种的缺电子性增强及溢流氢数量增多有关.

参考文献

[1] Bodnariuk P;Coq B;Ferrat G;Figueras F .[J].Journal of Catalysis,1989,116:459.
[2] Babu N S;Lingaiah N;Pasha N;Kumar J V Prasad P S S .[J].Catalysis Today,2009,141:120.
[3] Gopinath R;Lingaiah N;Sreedhar B;Suryanarayana I Prasad P S S Obuchi A .[J].Applied Catalysis B:Environmental,2003,46:587.
[4] Babu N S;Lingaiah N;Kumar J V;Prasad P S S .[J].Applied Catalysis A:General,2009,367:70.
[5] Juszczyk W;Malinowski A;Karpi(n)ski Z .[J].Applied Catalysis A:General,1998,166:311.
[6] 高燕,廖世健,徐杰,上官勇刚,顾志祥,蹇锡高.PVP-Pd催化六氯苯加氢脱氯中两种氢源的贡献[J].催化学报,2000(04):378-380.
[7] Chary KVR;Lakshmi KS;Rao PVR;Rao KSR;Papadaki M .Characterization and catalytic properties of niobia supported nickel catalysts in the hydrodechlorination of 1,2,4-trichlorobenzene[J].Journal of molecular catalysis, A. Chemical,2004(1/2):353-361.
[8] Pina G.;Louis C.;Keane MA. .Nickel particle size effects in catalytic hydrogenation and hydrodechlorination: phenolic transformations over nickel/silica[J].Physical chemistry chemical physics: PCCP,2003(9):1924-1931.
[9] Feng, J.-T.;Lin, Y.-J.;Evans, D.G.;Duan, X.;Li, D.-Q. .Enhanced metal dispersion and hydrodechlorination properties of a Ni/Al_2O_3 catalyst derived from layered double hydroxides[J].Journal of Catalysis,2009(2):351-358.
[10] de Lucas Consuegra A;Patterson P M;Keane M A .[J].Applied Catalysis B:Environmental,2006,65:227.
[11] Gryglewicz G;Stolarski M;Gryglewicz S;Klijanienko A;Piechocki W;Hoste S;Van Driessche I;Carleer R;Yperman J .Hydrodechlorination of dichlorobiphenyls over Ni-Mo/Al2O3 catalysts prepared by spray-drying method[J].Chemosphere: Environmental toxicology and risk assessment,2006(1):135-141.
[12] Liu X G;Chen J X;Zhang J Y .[J].Industrial and Engineering Chemistry Research,2008,47:5362.
[13] 周少君,陈吉祥,刘旭光,张继炎.还原条件对Ni2P/SiO2催化剂催化氯苯气相加氢脱氯反应性能的影响[J].催化学报,2007(06):498-500.
[14] 郭提,陈吉祥,李克伦.水蒸气处理对Ni2P/SiO2催化剂催化氯苯加氢脱氯反应的促进作用[J].催化学报,2012(07):1080-1085.
[15] Shen JH;Chen YW .Catalytic properties of bimetallic NiCoB nanoalloy catalysts for hydrogenation of p-chloronitrobenzene[J].Journal of molecular catalysis, A. Chemical,2007(1/2):265-276.
[16] Oyama S T;Wang X;Lee Y K;Bando K Requejo F G .[J].Journal of Catalysis,2002,210:207.
[17] Oyama S T;Wang X;Lee Y K;Chun W J .[J].Journal of Catalysis,2004,221:263.
[18] Lee Y K;Oyama S T .[J].Journal of Catalysis,2006,239:376.
[19] Kawai T;Bando K K;Lee Y K;Oyama S T,Chun W J.Asakura K.J C atal .[J].,2006,241:20.
[20] Layman K A;Bussell M E .[J].Journal of Physical Chemistry B,2004,108:10930.
[21] Sawhill SJ;Layman KA;Van Wyk DR;Engelhard MH;Wang C;Bussell ME .Thiophene hydrodesulfurization over nickel phosphide catalysts: effect of the precursor composition and support[J].Journal of Catalysis,2005(2):300-313.
[22] López E;Díez F V;Ordó(n)ez S .[J].Applied Catalysis B:Environmental,2008,82:264.
[23] Jang B W L;Spivey J J .[J].Catalysis Today,2000,55:3.
[24] Frimmel J.;Zdrazil M. .COMPARATIVE STUDY OF ACTIVITY AND SELECTIVITY OF TRANSITION METAL SULFIDES IN PARALLEL HYDRODECHLORINATION OF DICHLOROBENZENE AND HYDRODESULFURIZATION OF METHYLTHIOPHENE[J].Journal of Catalysis,1997(1):286-295.
[25] Murena F .[J].Journal of Hazardous Materials,2000,75:49.
[26] Ribeiro FH.;Rupprechter G.;Somorjai GA.;Kellner CS. Coulston GW.;Manzer LE.;Abrams L.;Gerken CA. .Structure insensitivity and effect of sulfur in the reaction of hydrodechlorination of 1,1-dichlorotetrafluoroethane (CF3-CFCl2) over Pd catalysts[J].Journal of Catalysis,1998(2):352-357.
[27] Li K L;Wang R J;Chen J X .[J].Energy and Fuels,2011,25:854.
[28] Nelson A E;Sun M;Junaid A S M .[J].Journal of Catalysis,2006,241:180.
[29] Chen J X;Zhou S J;Ci D H;Zhang J X Wang R J Zhang J Y .[J].Industrial and Engineering Chemistry Research,2009,48:3812.
[30] Murthy KV;Patterson P M;Jacobs G;Davis B H Keane M A .[J].Journal of Catalysis,2004,223:74.
[31] Zuzaniuk V;Prins R .[J].Journal of Catalysis,2003,219:85.
[32] Dufresne P;Payen E;Grimblot J;Bonnelle J P .[J].Journal of Physical Chemistry,1981,85:2344.
[33] Kiskinova M;Goodman D W .[J].Surface Science,1981,108:64.
[34] Conner W C;Falconer J L .[J].CHEMICAL REVIEWS,1995,95:759.
[35] Wojcieszak R;Monteverdi S;Mercy M;Nowak I Ziolek M Bettahar M M .[J].Applied Catalysis A:General,2004,268:241.
[36] Coq B;Ferrat G;Figueras F .[J].Journal of Catalysis,1986,101:434.
[37] Ordó(n)ez S;Díaz E;Bueres R F;Asedegbega-Nieto E Sastre H .[J].Journal of Catalysis,2010,272:158.
[38] Díaz E;Ordó(n)ez S;Bueres R F;Asedegbega-Nieto E Sastre H .[J].Applied Catalysis B:Environmental,2010,99:181.
[39] Nφrskov J K;Bligaard T;Logadottir A;Bahn S Hansen L B Bollinger M Bengaard H Hammer B Sljivancanin Z Mavrikakis M Xu Y Dahl S Jacobsen C J H .[J].Journal of Catalysis,2002,209:275.
[40] Liu P;Rodriguez J A;Asakura T;Gomes J Nakamura K .[J].Journal of Physical Chemistry B,2005,109:4575.
[41] Liu P;Rodriguez J A .[J].Catalysis Letters,2003,91:247.
[42] Gómez-Sainero L M;Seoane X L;Fierro J L G;Arcoya A .[J].Journal of Catalysis,2002,209:279.
[43] Bae JW;Lee JS;Lee KH .Hydrodechlorination of CCl4 over Pt/gamma-Al2O3 prepared from different pt precursors[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2008(1/2):156-167.
[44] Tφpsoe N Y;Tφpsoe H .[J].Journal of Catalysis,1993,139:641.
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%