将 HZSM-5 (n(SiO2)/n(Al2O3) = 25, 38, 50 和 93.5), HM, Hβ, HY 和γ-Al2O3 等多种固体酸催化剂用于二甲醚(DME)水解, 并将其分别同自制的 CuO/ZnO/Al2O3 催化剂进行机械混合, 制备双功能催化剂并用于 DME 水蒸气重整制氢反应. 结合 NH3 程序升温脱附表征手段, 考察了固体酸催化剂酸性位的强度、酸量及种类对 DME 水解和重整反应的影响;结合热重-差热扫描量热分析表征手段, 研究了 HZSM-5(93.5)和γ-Al2O3 在 DME 水解过程中的稳定性. 在此基础上, 进一步研究了固体酸催化剂对 DME 重整制氢反应中 DME 转化率、H2 摩尔产率以及含碳气体产物选择性的影响. 结果表明, 固体酸催化剂的酸性位的强度和酸量对 DME 重整制氢过程具有显著的影响, 强酸度和高酸量无益于 DME 水蒸气重整制氢;以 HZSM-5 为固体酸的双功能催化剂具有较好的低温活性, 而以γ-Al2O3 为固体酸的双功能催化剂在高温下具有较高的 H2 产率.
参考文献
[1] | 汤颖,刘晔,路勇,朱萍,何鸣元.CuZnAl水滑石衍生催化剂上甲醇水蒸气重整制氢Ⅰ.催化剂焙烧温度的影响[J].催化学报,2006(10):857-862. |
[2] | 王树东.[A].西安:西安交通大学出版社,2007:15. |
[3] | Zhou L;Guo Y;Zhang Q;Yagi M Li H B Chen J Sakurai M Kameyama H .[J].Catalysis Communications,2008,10:325. |
[4] | Jones S D;Neal L M;Hagelin-Weaver H E .[J].Applied Catalysis,2008,84:631. |
[5] | Wang H;Liu Y;Wang L;Qin Y N .[J].Chemical Engineering,2008,145:25. |
[6] | Yamada Y;Mathew T;Ueda A;Shioyama H Kobayashi T .[J].Applied Surface Science,2006,252:2593. |
[7] | Semelsberger T A;Borup R L;Greene H L .[J].Journal of Power Sources,2006,156:497. |
[8] | 王晓蕾,任克威,林瑞,潘相敏,马建新.二甲醚重整制氢技术的研究进展[J].天然气化工,2008(03):65-70. |
[9] | Zou J J;Zhang Y P;Liu C J .[J].Journal of Power Sources,2007,163:653. |
[10] | Tanaka Y;Kikuchi R;Takeguchi T;Eguchi K .[J].Applied Catalysis B:Environmental,2005,57:211. |
[11] | Fukunaga T;Ryumon N;Shimazu S .[J].Applied Catalysis A:General,2008,348:193. |
[12] | Semelsberger TA;Ott KC;Borup RL;Greene HL .Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using physical mixtures of a commercial Cu/Zn/Al2O3 catalyst and several solid-acid catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(3/4):291-300. |
[13] | Galvita V V;Semin G L;Belyaev V D;Yurieva T M Sobyanin V A .[J].Applied Catalysis A:General,2001,216:85. |
[14] | Nilsson M;Pettersson L J;Lindstr?m B .[J].Energy and Fuels,2006,20:2164. |
[15] | Faungnawakij K;Tanaka Y;Shimoda N;Fukunaga T;Kawashima S;Kikuchi R;Eguchi K .Influence of solid-acid catalysts on steam reforming and hydrolysis of dimethyl ether for hydrogen production[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(1):40-48. |
[16] | Faungnawakij K;Kikuchi R;Matsui T;Fukunaga T Eguchi K .[J].Applied Catalysis A:General,2007,333:114. |
[17] | Nishiguchi T;Oka K;Matsumoto T;Kanai H Utani K Imamura S .[J].Applied Catalysis A:General,2006,301:66. |
[18] | 汤颖,刘晔,路勇,朱萍,何鸣元.CuZnAl水滑石衍生催化剂上甲醇水蒸气重整制氢Ⅱ. 催化剂组成的影响[J].催化学报,2006(11):987-992. |
[19] | Takeishi K;Suzuki H .[J].Applied Catalysis A:General,2004,260:111. |
[20] | Kawabata T;Matsuoka H;Shishido T;Li DL;Tian Y;Sano T;Takehira K .Steam reforming of dimethyl ether over ZSM-5 coupled with Cu/ZnO/Al2O3 catalyst prepared by homogeneous precipitation[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):82-90. |
[21] | Matsumoto T;Nishiguchi T;Kanai H;Utani K;Matsumura Y;Imamura S .Steam reforming of dimethyl ether over H-mordenite-Cu/CeO2 catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2004(1/2):267-273. |
[22] | Mathew T;Yamada Y;Ueda A;Shioyama H;Kobayashi T .Metal oxide catalysts for DME steam reforming: Ga2O3 and Ga2O3-Al2O3 catalysts with and without copper[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2005(1):11-22. |
[23] | Faungnawakij K;Shimoda N;Fukunaga T;Kikuchi R Eguchi K .[J].Applied Catalysis A:General,2008,341:139. |
[24] | Semelsberger TA;Ott KC;Borup RL;Greene HL .Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using Cu/Zn supported on various solid-acid substrates[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(2):210-223. |
[25] | 宋凌珺,李兴虎,李聪,黄敏.二甲醚部分氧化重整制氢的实验研究[J].燃料化学学报,2008(01):79-82. |
[26] | Zou J J;Zhang Y P;Liu C J .[J].International Journal of Hydrogen Energy,2007,32:958. |
[27] | 冯冬梅;王金福;王德峥.[J].中国科技论文在线,2007 |
[28] | 余立挺,马建新.CuZnAlZr催化剂上甲醇氧化水蒸气重整制氢Ⅰ.催化剂组成的优化[J].催化学报,2004(07):523-528. |
[29] | Aboul-Gheit A K;Aboul-Gheit N A K;Awadallah A E .[J].催化学报,2008,29:113. |
[30] | Ramos F S;Duarte de Farias A M;Borges L E P;Monteiro J L Fraga M A Sousa-Aguiar E F Appel L G .[J].Catalysis Today,2005,101:39. |
[31] | Kiovsky J R;Goyette W J;Notermann T M .[J].Journal of Catalysis,1978,52:25. |
[32] | Vishwanathan V;Jun KW;Kim JW;Roh HS .Vapour phase dehydration of crude methanol to dimethyl ether over Na-modified H-ZSM-5 catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2004(1/2):251-255. |
[33] | Benito P L;Gayubo A G;Aguayo A T;Olazar M,Bilbao J .[J].Industrial and Engineering Chemistry Research,1996,35:3991. |
[34] | 宣东,沈晓春,楼辉,郑小明.不同方法制备的Zn/HZSM-5催化剂上甲烷和丙烷的无氧芳构化研究[J].浙江大学学报(理学版),2007(05):541-547. |
[35] | 张一卫,周钰明,邱安定,王玉,许艺,吴沛成.Na对PtSn/ZSM-5催化丙烷脱氢反应性能的影响[J].物理化学学报,2006(06):672-678. |
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%