以La_2O_3为载体,采用浸渍法制备了10%Ni/La_2O_3催化剂,考察了该催化剂的CO_2甲烷化反应性能.结果表明,在较低的温度(350℃)和高空速(约30000 h~(-1))下,甲烷时空收率可大于3000 g/(kg-h),无论转化率高低,甲烷选择性始终保持在100%.X射线衍射和H2-程序升温还原等表征结果表明,CO_2在Ni/La_2O_3催化剂上的加氢机理可能与Ni/γ-Al_2O_3上不同,并且La_2O_2CO_3的形成有利于提高催化剂活性.
The methanation of carbon dioxide on a Ni/La_2O_3 catalyst containing 10 wt% Ni prepared by the impregnation method was studied. The space-time yield of methane was 3000 g/(kg-h) at conditions of 350 ℃, GHSV of 30000 h~-1, 1.5 MPa pressure, and H_2/CO_2 molar ratio of 4/1. The selectivity for methane was 100% with different CO_2 conversions. Combined with X-ray diffraction and H_2 temperature-programmed reduction analyses, this suggested that the reaction mechanism on Ni/La_2O_3 may be different from that on Ni/γ-Al_2O_3. The formation of lanthanum oxycarbonate (La_2O_2CO_3) can play an important role in the activation of CO_2.
参考文献
| [1] | Alstrup I .[J].Journal of Catalysis,1998,151:216. |
| [2] | Sehested J;Dahl S;Jacobsen J;Rostrup-Nielsen J R .[J].Journal of Physical Chemistry B,2005,109:2432. |
| [3] | Hashimoto K.;Yamasaki M.;Meguro S.;Sasaki T.;Katagiri H. Matsui T.;Fujimura K.;Izumiya K.;Kumagai N.;Akiyama E.;Habazaki H. .Advanced materials for global carbon dioxide recycling[J].Materials Science & Engineering, A. Structural Materials: Properties, Misrostructure and Processing,2001(0):88-96. |
| [4] | Darensbourg D J;Bauch C G;Ovalles C .[J].Reviews in Inorganic Chemistry,1985,7:315. |
| [5] | Schild C;Wokaun A;Koppel R A;Baiker A .[J].Journal of Physical Chemistry,1991,95:6341. |
| [6] | Weatherbee G D;Bartholomew C H .[J].Journal of Catalysis,1982,77:460. |
| [7] | Du G A;Lim S Y;Yang Y H;Wang C Pfefferle L Haller G L .[J].Journal of Catalysis,2007,249:370. |
| [8] | Xiong K;Robertson J .[J].Microelectronic Engineering,2009,86:1672. |
| [9] | 魏树权;李丽波;商永臣;徐恒泳 徐国林 .[J].天然气化工,2004,29(10) |
| [10] | 邓庚风;郭年祥;罗来涛;李风仪 .[J].稀土,2002,23:18. |
| [11] | 郭芳,储伟,徐慧远,张涛.采用等离子体强化制备CO2甲烷化用镍基催化剂[J].催化学报,2007(05):429-434. |
| [12] | Lai T L;Shu Y Y;Huang G L;Lee C C Wang C B .[J].Journal of Alloys and Compounds,2008,450:318. |
| [13] | 黄继民,沈雷军,韩莉,谭润华.La2O3在空气中稳定性的研究[J].稀土,2002(03):72-73. |
| [14] | Squire G D;Luc H;Puxley D C .[J].Applied Catalysis A:General,1994,108:261. |
| [15] | Vesseili E;De Rogatis L;Ding X L;Baraldi A Savio L Vattuone L Rocca M Fornasiero P Peressi M Baldereschi A Rosei R Comelli G .[J].Journal of the American Chemical Society,2008,130:11417. |
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