分别采用溶胶-凝胶法、旋转蒸发微波干燥法、共沉淀法、浸渍法和机械混合法制备Ni-Mo氧化物前驱体。以H2和N2的混合气为氮化气体，采用程序升温氮化法合成了镍钼氮化物催化剂。利用X射线衍射、总氮含量分析、X射线光电子能谱及H2程序升温还原对Ni-Mo氧化物前体及氮化物催化剂进行了表征。将上述Ni-Mo氮化物催化剂用于丙烷氨氧化反应中。结果表明， Ni-Mo氧化物前驱体的制备方法影响其氮化物催化剂上丙烷氨氧化反应性能。 Ni-Mo氮化物催化剂中氮物种的移动性及反应性对产物丙烯腈选择性的影响较大，共沉淀法制备的催化剂存在大量的活性氮物种，因而具有良好的催化丙烷氨氧化反应活性。
Five different methods were used to prepare the Ni-Mo oxide precursors including sol-gel, rotary evaporation-microwave drying, co-precipitation, impregnation, and mechanical mixing. Ni-Mo ni-tride catalysts have been synthesized by temperature-programmed nitration of the oxide precur-sors in a flow of H2 and N2. The structure and physico-chemical properties of the Ni-Mo oxide pre-cursors and their corresponding nitride catalysts were determined by X-ray diffraction, total nitro-gen content analysis, X-ray photoelectron spectroscopy and H2 temperature-programmed reduc-tion, and their catalytic performance for propane ammoxidation was also tested. The catalytic activ-ity and selectivity towards the formation of acrylonitrile over the Ni-Mo nitride catalysts are strongly dependent on the preparation methods for the oxide precursors. The N species in the Ni-Mo nitrides and their mobility and reactivity affect the selectivity for acrylonitrile. The Ni-Mo nitride prepared by co-precipitation, with the largest amount and more reactive N species, exhibited the highest catalytic activity and selectivity for acrylonitrile.
参考文献
| [1] | Korlann S.;Diaz B.;Bussell ME. .Synthesis of bulk and alumina-supported bimetallic carbide and nitride catalysts[J].Chemistry of Materials,2002(10):4049-4058. |
| [2] | Volpe L;Boudart M .[J].Journal of Physical Chemistry,1986,90:4874. |
| [3] | Liang C H;Li W Z;Wei Z B;Xin Q Li C .[J].Industrial and Engineering Chemistry Research,2000,39:3694. |
| [4] | Zheng W Q;Cotter T P;Kaghazchi P;Jacob T Frank B Schlichte K Zhang W Su D S Schuth F Schlogl R .[J].Journal of the American Chemical Society,2013,135:3458. |
| [5] | Andonova S;Vladov C;Kunev B;Mitov I;Tyuliev G;Fierro JLG;Damyanova S;Petrov L .Study of the effect of mechanical-chemical activation of Co-Mo/gamma-Al2O3 and Ni-Mo/gamma-Al2O3 catalysts for hydrodesulfurization[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):94-102. |
| [6] | Monnier J;Sulimma H;Dalai A;Caravaggio G .[J].Applied Catalysis A:General,2010,382:176. |
| [7] | Hunter S M;Mckay D;Smith R I;Hargreaves J S J Gregory D H .[J].CHEMISTRY OF MATERIALS,2010,22:2898. |
| [8] | Hunter S M;Gregory D H;Hargreaves J S J;Richard M Duprez D Bion N .[J].ACS Catal,2013,3:1719. |
| [9] | 丁姜宏,徐乐,徐浩,吴海虹,刘月明,吴鹏.Ti-MOR钛硅分子筛催化甲乙酮氨氧化反应性能[J].催化学报,2013(01):243-250. |
| [10] | 姜枫,邓生财,牛磊,肖国民.载体对钒铬氧化物催化剂结构及催化3-甲基吡啶氨氧化反应活性的影响[J].催化学报,2013(10):1833-1838. |
| [11] | Li XK;Ji WH;Zhao J;Zhang Z;Au CT .A comparison study on the partial oxidation of n-butane and propane over VPO catalysts supported on SBA-15, MCM-41, and fumed SiO2[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):8-16. |
| [12] | Wickman A;Andersson A .[J].Applied Catalysis A:General,2011,391:110. |
| [13] | Pyrz W D;Blom D A;Vogt T;Buttrey D J .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2008,47:2788. |
| [14] | Shiju N R;Guliants V V .[J].CATALYSIS COMMUNICATIONS,2008,9:2253. |
| [15] | Safonova, O.V.;Florea, M.;Bilde, J.;Delichere, P.;Millet, J.M.M. .Local environment of vanadium in V/Al/O-mixed oxide catalyst for propane ammoxidation: Characterization by in situ valence-to-core X-ray emission spectroscopy and X-ray absorption spectroscopy[J].Journal of Catalysis,2009(1):156-164. |
| [16] | Sadakane M;Kodato K;Kuranishi T;Nodasaka Y Sugawara K Sakaguchi N Nagai T Matsui Y Ueda W .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2008,47:2493. |
| [17] | Zhang H M;Zhao Z;Xu C M;Duan A J .[J].CHEMISTRY LETTERS,2006,35:36. |
| [18] | Derouane-Abd Hamid S B;Pal P;He H Y;Derouane E G .[J].Catalysis Today,2001,64:129. |
| [19] | Centi G;Perathoner S;Trifirò F .[J].Applied Catalysis A:General,1997,157:143. |
| [20] | Olea M;Florea M;Sack I;Silvy RP;Gaigneaux EM;Marin GB;Grange P .Evidence for the participation of lattice nitrogen from vanadium aluminum oxynitrides in propane ammoxidation[J].Journal of Catalysis,2005(1):152-160. |
| [21] | Jacobsen C J H;Zhu J J;Lindel?v H;Jiang J Z .[J].Journal of Materials Chemistry,2002,12:3113. |
| [22] | Weil K S;Kumta P N;Grins J .[J].Journal of Solid State Chemistry,1999,146:22. |
| [23] | Wang H M;Li W;Zhang M H .[J].CHEMISTRY OF MATERIALS,2005,17:3262. |
| [24] | Markel E J;Van Zee J W .[J].Journal of Catalysis,1990,126:643. |
| [25] | Choi J G;Curl R L;Thompson L T .[J].Journal of Catalysis,1994,146:218. |
| [26] | Wise R S;Markel E J .[J].Journal of Catalysis,1994,145:344. |
| [27] | Guyader J;Grekov F F;Marchand R;Lang J .[J].REVUE DE CHIMIE MINERALE,1978,15:431. |
| [28] | Herle PS.;Sooryanarayana K.;Row TNG.;Subbanna GN.;Hegde MS. .Ni2Mo3N: A new ternary interstitial nitride with a filled beta-manganese structure[J].Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics,1998(16):4128-4130. |
| [29] | 张惠民,赵震.制备方法对Ni-Mo氧化物催化剂晶相结构的影响[J].工业催化,2008(09):34-36. |
| [30] | Cárdenas-Lizana F;Lamey D;Perret N;Gómez-Quero S Kiwi-Minsker L Keane M A .[J].CATALYSIS COMMUNICATIONS,2012,21:46. |
| [31] | Wang Y H;Li W;Zhang M H;Guan N J Tao K Y .[J].Applied Catalysis A:General,2001,215:39. |
| [32] | Colling C W;Thompson L T .[J].Journal of Catalysis,1994,146:193. |
| [33] | Levin D;Ying J Y .[J].Journal of Electroceramics,1999,3:25. |
| [34] | Zhang, QH;Cao, CJ;Xu, T;Sun, M;Zhang, JH;Wang, Y;Wan, HL .NiO-polyoxometalate nanocomposites as efficient catalysts for the oxidative dehydrogenation of propane and isobutane[J].Chemical communications,2009(17):2376-2378. |
| [35] | Chen JG. .SELECTIVE ACTIVATION OF C-H AND C=C BONDS ON METAL CARBIDES - A COMPARISON OF REACTIONS OF N-BUTANE AND 1,3-BUTADIENE ON VANADIUM CARBIDE FILMS ON V(110)[J].Journal of Catalysis,1995(1):80-90. |
| [36] | Ghampson I T;Sepúlveda C;Garcia R;Fierro J L G Escalona N DeSisto W J .[J].Applied Catalysis A:General,2012,435-436:51. |
| [37] | Nagai M;Takada J;Omi S .[J].Journal of Physical Chemistry B,1999,103:10180. |
| [38] | Yao Z W;Zhang A J;Li Y;Zhang Y Z Cheng X Q Shi C .[J].Journal of Alloys and Compounds,2008,464:488. |
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