采用程序升温还原方法制备了Ni2P/SiO2催化剂,考察了还原条件对催化剂结构及其催化氯苯加氢脱氯反应性能的影响.结果表明,还原条件(氢气流速、还原温度及时间)对Ni2P/SiO2催化剂的比表面积、孔结构及Ni2P晶粒大小没有明显的影响,但催化剂表面的磷含量差异较大.Ni2P/SiO2催化剂在氯苯加氢脱氯反应过程中存在一定的诱导期,而采用提高还原温度和H2空速以及延长还原时间等方法制备的催化剂可以缩短反应诱导期.初步分析认为磷覆盖催化剂活性中心是产生诱导期的主要原因,而还原条件会影响催化剂的表面性质.Ni2P/SiO2催化剂具有良好的加氢脱氯活性及稳定性,在573 K,H2流量75 ml/min及氯苯流量3 ml/h的条件下,该催化剂上氯苯转化率在130 h内保持在99%以上.
参考文献
[1] | Sweeny N P;Rohrer C S;Brown O W .[J].Journal of the American Chemical Society,1958,80(04):799. |
[2] | Nozaki F;Adachi R .[J].Journal of Catalysis,1975,40(02):166. |
[3] | Phillips D C;Sawhill S J;Self R;Bussell M E .[J].Journal of Catalysis,2002,207(02):266. |
[4] | 孙福侠,魏昭彬,应品良,孙秀萍,蒋宗轩,田福平,杨永兴,李灿.一种新型高活性加氢脱硫催化剂:二氧化硅担载的磷化镍[J].催化学报,2004(09):685-687. |
[5] | Yang Sh F;Liang Ch H;Prins R .[J].Journal of Catalysis,2006,237(01):118. |
[6] | 宋立民,李伟,张明慧,陶克毅.由非晶态Ni-P低温制备Ni2P催化剂及其对二苯并噻吩加氢脱硫的催化性能[J].催化学报,2006(12):1127-1132. |
[7] | Lee Y-K;Shu Y Y;Oyama S T .[J].Applied Catalysis A:General,2007,322:191. |
[8] | Stinner C;Prins R;Weber Th .[J].Journal of Catalysis,2001,202(01):187. |
[9] | Oyama S T;Wang X;Lee Y-K;Chun W-J .[J].Journal of Catalysis,2004,221(02):263. |
[10] | Keane M A .[J].Applied Catalysis A:General,2004,271(1-2):109. |
[11] | Wu W H;Xu J;Ohnishi R .[J].Applied Catalysis B:Environmental,2005,60(1-2):129. |
[12] | Calvo L;Gilarranz MA;Casas JA;Mohedano AF;Rodriguez JJ .Hydrodechlorination of 4-chlorophenol in aqueous phase using Pd/AC catalysts prepared with modified active carbon supports[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(1/2):68-76. |
[13] | Liu X G;Chen J X;Zhang J Y.[J].CATALYSIS COMMUNICATIONS |
[14] | Oyama S T;Wang X;Lee Y-K;Bando K Requejo F G .[J].Journal of Catalysis,2002,210(01):207. |
[15] | Lee Y-K;Oyama S T .[J].Journal of Catalysis,2006,239(02):376. |
[16] | Sawhill SJ.;Phillips DC.;Bussell ME. .Thiophene hydrodesulfurization over supported nickel phosphide catalysts[J].Journal of Catalysis,2003(2):208-219. |
[17] | 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. |
[18] | Stinner C.;Tang Z.;Haouas M.;Weber T.;Prins R. .Preparation and P-31 NMR characterization of nickel phosphides on silica[J].Journal of Catalysis,2002(2):456-466. |
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:
-
10%
-
20%
-
30%
-
40%
-
50%