介孔型铝酸镍纳米棒的制备及其催化氢化裂解甲苯性能

doi:10.3866/PKU.WHXB20110711

物理化学学报 >> 2011, Vol. 27 >> Issue (07): 1743-1750.doi: 10.3866/PKU.WHXB20110711

介孔型铝酸镍纳米棒的制备及其催化氢化裂解甲苯性能

申杉杉, 陆文聪, 张良苗, 岳宝华, 韩玲, 张浩

上海大学化学系, 上海 200444

收稿日期:2011-02-23 修回日期:2011-05-05 发布日期:2011-06-28
通讯作者: 陆文聪 E-mail:wclu@shu.edu.cn
基金资助:
国家自然科学基金(20973108), 上海教委(11ZZ83), 上海市重点学科建设 (J50101)和上海大学创新基金(A.10-0101-09-023)资助项目

Fabrication of Mesoporous NiAl₂O₄ Nanorods and Their Catalytic Properties for Toluene Hydrocracking

SHEN Shan-Shan, LU Wen-Cong, ZHANG Liang-Miao, YUE Bao-Hua, HAN Ling, ZHANG Hao

Department of Chemistry, Shanghai University, Shanghai 200444, P. R. China

Received:2011-02-23 Revised:2011-05-05 Published:2011-06-28
Contact: LU Wen-Cong E-mail:wclu@shu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20973108), Shanghai Education Committee, China (11ZZ83), Shanghai Leading Academic Discipline Project, China (J50101), and Innovation Fund of Shanghai University, China (A.10-0101-09-023).

摘要/Abstract

摘要：

以NH₄HCO₃为造孔剂通过一步水热法成功合成了介孔型单晶NiAl₂O₄纳米棒, 并考察了不同反应条件对NiAl₂O₄形貌的影响. 实验结果表明反应时间、反应物浓度、NH₄HCO₃加入量对产物形貌具有关键作用. 用透射电子显微镜(TEM), 高分辨透射电子显微镜(HRTEM), 扫描电子显微镜(SEM)和X射线衍射仪(XRD)对NiAl₂O₄纳米棒的形貌、结构和组成进行表征, 并用氮气吸附-脱附法对其比表面积和孔径分布进行了研究. 以介孔型NiAl₂O₄纳米棒为催化剂, 在固定床反应器上对甲苯进行催化实验, 结果表明当水炭摩尔比为1.0、反应温度为700 ℃时, 400 min反应时间内甲苯平均转化率高达86.5%, 并具有较好的反应稳定性. 比较了直接沉淀法制备的纳米颗粒作为催化剂在甲苯氢化催化裂解中的催化性能. 结果表明水热法制备的棒状NiAl₂O₄催化剂比不用水热制备的催化剂催化活性要好. 初步探讨了介孔型NiAl₂O₄纳米棒的可能形成机理.

关键词: 水热法, 单晶NiAl₂O₄, NH₄HCO₃, 镍基催化剂, 表征

Abstract:

Mesoporous single-crystalline NiAl₂O₄ nanorods were successfully synthesized by a one-step hydrothermal method using a pore-forming agent (NH₄HCO₃). A series of controlled experiments were also carried out to better understand the formation mechanism of NiAl₂O₄ nanorods. The experimental results indicate that the reaction time, reactant concentration and the amount of NH₄HCO₃ play an important role in determining the morphology. The morphology, structure and composition of the nanorods were investigated using transmission electron microscopy, high resolution transmission electron microscopy, scanning electron microscopy and X-ray diffraction. The specific surface area and pore-size distribution of the obtained product was determined by nitrogen adsorption-desorption measurements. NiAl₂O₄ nanorods have a high Brunauer-Emmett-Teller surface area and good porosity properties. The catalytic performance of the NiAl₂O₄ nanorods during toluene hydrocracking was investigated using a fixed bed reactor. After the toluene catalytic reactions over 400 min at a water stream/carbon molar ratio (H₂O/C) of 1.0 with a reaction temperature of 700 ℃ the average conversion efficiency of toluene was about 86.5%. Compared to the NiAl₂O₄ nanoparticles prepared by alkaline precipitation, the mesoporous NiAl₂O₄ nanorods exhibited higher catalytic activity and stability during toluene hydrocracking. A possible formation mechanism for the mesoporous NiAl₂O₄ nanorods is proposed and discussed.

Key words: Hydrothermal method, Single-crystalline NiAl₂O₄, NH₄HCO₃, Nickel catalyst, Characterization

申杉杉, 陆文聪, 张良苗, 岳宝华, 韩玲, 张浩. 介孔型铝酸镍纳米棒的制备及其催化氢化裂解甲苯性能[J]. 物理化学学报, 2011, 27(07): 1743-1750.

SHEN Shan-Shan, LU Wen-Cong, ZHANG Liang-Miao, YUE Bao-Hua, HAN Ling, ZHANG Hao. Fabrication of Mesoporous NiAl₂O₄ Nanorods and Their Catalytic Properties for Toluene Hydrocracking[J]. Acta Phys. -Chim. Sin., 2011, 27(07): 1743-1750.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110711

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I07/1743

参考文献

(1) Buffoni, I. N.; Pompeo, F.; Santori, G. F.; Nichio, N. N. Catalysis Communications 2009, 10, 1656.
(2) Wu, M. X.; Li,W.; Zhang, M. H.; Tao, K. Y. Acta Physico-Chimica Sinica 2007, 23, 1311. [武美霞, 李伟, 张明慧, 陶克毅. 物理化学学报, 2007, 23, 1311.]
(3) Seo, J. G.; Youn, M. H.; Song, I. K. Catalysis Surveys from Asia 2010, 14, 1.
(4) Yolcular, S.; Olgun, O. Catalysis Today 2008, 138, 198.
(5) Muroyama, H.; Nakase, R.; Matsui, T.; Eguchi, K. International Journal of Hydrogen Energy 2010, 35, 1575.
(6) Valentini, A.; Carre?o, N. L. V.; Probst, L. F. D.; Leite, E. R.; Longo, E. Microporous and Mesoporous Materials 2004, 68, 151.
(7) Sivaiah, M. V.; Petit, S.; Beaufort, M. F.; Eyidi, D.; Barrault, J.; Batiot-Dupeyrat, C.; Valange, S. Microporous and Mesoporous Materials, 2011, 140, 69.
(8) Popov, A. G.; Smirnov, A. V.; Knyazeva, E. E.; Yuschenko, V. V.; Kalistratova, E. A.; Klementiev, K. V.; Grünert,W.; Ivanova, I. I. Microporous and Mesoporous Materials 2010, 134, 124.
(9) Yue, B.;Wang, X.; Ai, X.; Yang, J.; Li, L.; Lu, X.; Ding,W. Fuel Processing Technology 2010, 91, 1098.
(10) Cheng, H.W.; Zhang, Y.W.; Lu, X. G.; Ding,W. Z.; Li, Q. Energy & Fuels 2009, 23, 414.
(11) Song, X. C.; Zheng, Y. F.; Lin, S.;Wang, Y. Acta Physico-Chimica Sinica 2007, 23, 258. [宋旭春, 郑遗凡, 林深, 王芸. 物理化学学报, 2007, 23, 258.]
(12) Chen, A. M.; Xu, S. F.; Ni, Z. M. Acta Physico-Chimica Sinica 2009, 25, 2570. [陈爱民, 徐淑芬, 倪哲明. 物理化学学报, 2009, 25, 2570.]
(13) Chen, J. H.; Xue, C. S.; Zhuang, H. Z.; Li, H.; Qin, L. X.; Yang, Z. Z. Acta Physico-Chimica Sinica 2008, 24, 355. [陈金华, 薛成山, 庄惠照, 李红, 秦丽霞, 杨兆柱. 物理化学学报, 2008, 24, 355.]
(14) Vijaya, J. J.; Kennedy, L. J.; Sekaran, G.; Nagaraja, K. S. Materials Letters 2007, 61, 5213.
(15) Amini, M. M.; Torkian, L. Materials Letters 2002, 57, 639.
(16) Pettit, F. S.; Randklev, E. H.; Felten, E. J. Journal of the American Ceramic Society 1966, 49, 199.
(17) Platero, E. E.; Arean, C. O.; Parra, J. B. Research on Chemical Intermediates 1999, 25, 187.
(18) Zangouei, M.; Moghaddam, A. Z.; Razeghi, A.; Omidkhah, M. R. International Journal of Chemical Reactor Engineering 2010, 8, S1.
(19) Yung, M. M.; Magrini-Bair, K. A.; Parent, Y. O.; Carpenter, D. L.; Feik, C. J.; Gaston, K. R.; Pomeroy, M. D.; Phillips, S. D. Catalysis Letters 2010, 134, 242.
(20) Gama, L.; Ribeiro, M. A.; Barros, B. S.; Kiminami, R. H. A.; Weber, I. T.; Costa, A. C. F. M. Journal of Alloys and Compounds 2009, 483, 453.
(21) Nogueira, N. A. S.; da Silva, E. B.; Jardim, P. M.; Sasaki, J. M. Materials Letters 2007, 61, 4743.
(22) Kanthimathi, M.; Dhathathreyan, A.; Nair, B. Materials Letters 2004, 58, 2914.
(23) Velu, S.; Shah, N.; Jyothi, T. M.; Sivasanker, S. Microporous and Mesoporous Materials 1999, 33, 61.
(24) Kim, H.W.; Kang, K. M.; Kwak, H. Y. International Journal of Hydrogen Energy 2009, 34, 3351.
(25) Romero, A.; Jobbagy, M.; Laborde, M.; Baronetti, G.; Amadeo, N. Catalysis Today 2010, 149, 407.
(26) Voorhees, P. Journal of Statistical Physics 1985, 38, 231.
(27) Zhao, Z.; Zhang, L.; Dai, H.; Du, Y.; Meng, X.; Zhang, R.; Liu, Y.; Deng, J. Microporous and Mesoporous Materials 2011, 138, 191.
(28) Whitesides, G.; Mathias, J.; Seto, C. Science 1991, 254, 1312.
(29) Zhang, L.; Lu,W.; Yan, L.; Feng, Y.; Bao, X.; Ni, J.; Shang, X.; Lv, Y. Microporous and Mesoporous Materials 2009, 119, 208.
(30) Liu, J.; Harris, A. T. AICHE Journal 2010, 56, 102.
(31) Zhang, S. M.; Zeng, H. C. Chemistry of Materials 2009, 21, 871.
(32) Mavis, B.; Akinc, M. Chemistry of Materials 2006, 18, 5317.
(33) Osaki, T.; Horiuchi, T.; Sugiyama, T.; Suzuki, K.; Mori, T. Catalysis Letters 1998, 52, 171.
(34) Saadi, A.; Merabiti, R.; Rassoul, Z.; Bettahar, M. M. Journal of Molecular Catalysis A-Chemical 2006, 253, 79.
(35) Zhao, J.; He, X.;Wang, L.; Tian, J.;Wan, C.; Jiang, C. International Journal of Hydrogen Energy 2007, 32, 380.
(36) Oyama, S. T.; Lee, Y. K. Journal of Catalysis 2008, 258, 393.
(37) Shigarov, A. B.; Kireenkov, V. V.; Kuzmin, V. A.; Kuzin, N. A.; Kirillov, V. A. Catalysis Today 2009, 144, 341.

[1]	胡洋, 刘斌, 徐路遥, 董自强, 仵亚婷, 刘杰, 钟澄, 胡文彬. 基于微流控技术平台的Pt基三元电催化剂高通量合成和筛选[J]. 物理化学学报, 2023, 39(3): 2209004 -0 .
[2]	莫英, 肖逵逵, 吴剑芳, 刘辉, 胡爱平, 高鹏, 刘继磊. 锂离子电池隔膜的功能化改性及表征技术[J]. 物理化学学报, 2022, 38(6): 2107030 - .
[3]	黄俊达, 朱宇辉, 冯煜, 韩叶虎, 谷振一, 刘日鑫, 杨冬月, 陈凯, 张相禹, 孙威, 辛森, 余彦, 尉海军, 张旭, 于乐, 王华, 刘新华, 付永柱, 李国杰, 吴兴隆, 马灿良, 王飞, 陈龙, 周光敏, 吴思思, 卢周广, 李秀婷, 刘继磊, 高鹏, 梁宵, 常智, 叶华林, 李彦光, 周亮, 尤雅, 王鹏飞, 杨超, 刘金平, 孙美玲, 毛明磊, 陈浩, 张山青, 黄岗, 余丁山, 徐建铁, 熊胜林, 张进涛, 王莹, 任玉荣, 杨春鹏, 徐韵涵, 陈亚楠, 许运华, 陈子峰, 杲祥文, 浦圣达, 郭少华, 李强, 曹晓雨, 明军, 皮欣朋, 梁超凡, 伽龙, 王俊雄, 焦淑红, 姚雨, 晏成林, 周栋, 李宝华, 彭新文, 陈冲, 唐永炳, 张桥保, 刘奇, 任金粲, 贺艳兵, 郝晓鸽, 郗凯, 陈立宝, 马建民. 二次电池研究进展[J]. 物理化学学报, 2022, 38(12): 2208008 - .
[4]	周雪梅. 二氧化钛负载单原子催化剂用于光催化反应的研究[J]. 物理化学学报, 2021, 37(6): 2008064 - .
[5]	岳昕阳, 马萃, 包戬, 杨思宇, 陈东, 吴晓京, 周永宁. 金属锂负极失效机制及其先进表征技术[J]. 物理化学学报, 2021, 37(2): 2005012 - .
[6]	王晗, 安汉文, 单红梅, 赵雷, 王家钧. 全固态电池界面的研究进展[J]. 物理化学学报, 2021, 37(11): 2007070 - .
[7]	潘弘毅, 李泉, 禹习谦, 李泓. 多空间尺度下的金属锂负极表征技术[J]. 物理化学学报, 2021, 37(1): 2008091 - .
[8]	史永超, 唐明学. 可充电池的磁共振研究[J]. 物理化学学报, 2020, 36(4): 1905004 - .
[9]	刘璐, 徐玉萍, 陈霞, 洪梅, 佟静. 1-烷基-3-甲基咪唑氯化物焓变的热重分析[J]. 物理化学学报, 2020, 36(11): 2004014 - .
[10]	赵华博, 马丁. χ-Fe₅C₂：结构，合成与催化性质调控[J]. 物理化学学报, 2020, 36(1): 1906087 - .
[11]	卢秀利,韩莹莹,鲁统部. 石墨炔结构表征及在光电催化反应中的应用[J]. 物理化学学报, 2018, 34(9): 1014 -1028 .
[12]	陈凡,王中跃,张艳艳,余柯涵,翁丽星,韦玮. 聚丙烯酸功能化高效发光的La_1-xEu_xF₃纳米晶合成及细胞成像[J]. 物理化学学报, 2017, 33(7): 1446 -1452 .
[13]	高晓平,郭章龙,周亚男,敬方梨,储伟. 锐钛矿型TiO₂担载的Pd催化剂用于乙炔选择加氢的催化性能及其表征[J]. 物理化学学报, 2017, 33(3): 602 -610 .
[14]	李申慧,李静,郑安民,邓风. 固体酸催化剂结构与催化反应机理的核磁共振研究[J]. 物理化学学报, 2017, 33(2): 270 -282 .
[15]	张晓茹,许跃峰,沈守宇,陈媛,黄令,李君涛,孙世刚. 锂氧电池双功能还原石墨烯-LaFeO₃复合纳米催化剂的制备及性能[J]. 物理化学学报, 2017, 33(11): 2237 -2244 .

介孔型铝酸镍纳米棒的制备及其催化氢化裂解甲苯性能

Fabrication of Mesoporous NiAl₂O₄ Nanorods and Their Catalytic Properties for Toluene Hydrocracking

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

推荐阅读 0

介孔型铝酸镍纳米棒的制备及其催化氢化裂解甲苯性能

Fabrication of Mesoporous NiAl2O4 Nanorods and Their Catalytic Properties for Toluene Hydrocracking

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

推荐阅读 0

Fabrication of Mesoporous NiAl₂O₄ Nanorods and Their Catalytic Properties for Toluene Hydrocracking