以MnSO_4和KMnO_4为前驱体,采用回流法在酸性介质中合成了氧化锰八面体分子筛(OMS-2).以OMS-2为载体采用浸渍法制备了PdO/OMS-2催化剂,并对催化剂进行了表征和CO氧化活性测试.结果表明,OMS-2为纳米棒结构,是典型的隐钾锰矿(cryptomelane)结构.当PdO负载量≤1.0%时,PdO以高分散的形式存在,而更高负载量时形成PdO晶相.当PdO负载量为2.5%时,PdO/OMS-2催化剂上CO氧化反应活性最高,CO完伞转化温度为80℃.催化剂中高分散的PdO和高价态的Pd物种是反应的活性中心.
A manganese oxide octahedral molecular sieve (OMS-2) was synthesized using MnSO_4 and KMnO_4 as precursors by a reflux method under acidic conditions. PdO supported on OMS-2 (PdO/OMS-2) was prepared and tested for CO oxidation. The results showed that the OMS-2 molecular sieve was in the form of nano-rods and had typical structure with cryptomelane. PdO was highly dispersed when the PdO loading was lower than 1.0%, while crystalline PdO formed at higher PdO loading. The 2.5%PdO/OMS-2 catalyst was most active for CO oxidation with 100% conversion of CO at 80 ℃. The highly dispersed PdO species and Pd species with high oxidation state were the active sites for the reaction.
参考文献
[1] | Yuan YZ.;Asakura K.;Wan HL.;Tsai K.;Iwasawa Y.;Kozlova AP. .SUPPORTED AU CATALYSTS PREPARED FROM AU PHOSPHINE COMPLEXES AND AS-PRECIPITATED METAL HYDROXIDES - CHARACTERIZATION AND LOW-TEMPERATURE CO OXIDATION[J].Journal of Catalysis,1997(1):191-199. |
[2] | Luo M F;Pu Z Y;He M;Jin J Jin L Y .[J].Journal of Molecular Catalysis A:Chemical,2006,260:152. |
[3] | Faticanti M;Cioffi N;De Rossi S;Ditaranto N Porta P Sabbatini L Bleve-Zacheo T .[J].Applied Catalysis B:Environmental,2005,60:73. |
[4] | DeGuzman R N;Shen Y F;Neth E J;Suib S L O'Young C L Levine S Newsam J M .[J].Chemistry of Materials,1994,6:815. |
[5] | Luo J;Zhang Q H;Huang A M;Suib S L .[J].Microporous and Mesoporous Materials,2000,35-36:209. |
[6] | Gandhe AR;Rebello JS;Figueiredo JL;Fernandes JB .Manganese oxide OMS-2 as an effective catalyst for total oxidation of ethyl acetate[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(1/2):129-135. |
[7] | Chen J L;Li J;Li H J;Huang X M Shen W J .[J].Microporous and Mesoporous Materials,2008,116:586. |
[8] | 胡蓉蓉,程易,XIE Lanying,谢兰英,王德峥.掺Ag对氧化锰八面体分子筛催化CO氧化性能的影响[J].催化学报,2007(05):463-468. |
[9] | Chen X.;Shen YF.;Suib SL.;O'Young CL. .Characterization of manganese oxide octahedral molecular sieve (M-OMS-2) materials with different metal cation dopants[J].Chemistry of Materials,2002(2):940-948. |
[10] | de la Pe(n)a O'Shea V A;(A)lvarez-Galv(a)na M C;Fierroa J L G;Arias P L .[J].Applied Catalysis B:Environmental,2005,57:191. |
[11] | Tang X F;Li Y G;Huang X M;Xu Y D,Zhu H Q,Wang J G,Shen W J .[J].Applied Catalysis B:Environmental,2006,62:265. |
[12] | Luo J Y;Meng M;Yao J S;Li X G Zha Y Q Wang X T Zhang T Y .[J].Applied Catalysis B:Environmental,2009,87:92. |
[13] | 周仁贤.氧化铈对Pd/Al2O3表面上CO氧化性能的影响[J].高等学校化学学报,1996(03):443. |
[14] | Cimino S;Casaletto M P;Lisi L;Russo G .[J].Applied Catalysis A:General,2007,327:238. |
[15] | Gac W .[J].Applied Catalysis B:Environmental,2007,75:107. |
[16] | Xia G G;Yin Y G;Willis W S;Wang J Y Suib S L .[J].Journal of Catalysis,1999,185:91. |
[17] | Xu R;Wang X;Wang D S;Zhou K B Li Y D .[J].Journal of Catalysis,2006,237:426. |
[18] | Faticanti M;Cioffi N;Rossi S D;Ditaranto N Porta P Sabbatini L Bleve-Zacheo T .[J].Applied Catalysis B,2005,60:73. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%