Dispersion of copper species in a confined space and their application in thiophene capture

被引:90
作者
Yin, Yu [1 ]
Jiang, Wen-Juan [1 ]
Liu, Xiao-Qin [1 ]
Li, Yan-Hua [1 ]
Sun, Lin-Bing [1 ]
机构
[1] Nanjing Univ Technol, Coll Chem & Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 210009, Jiangsu, Peoples R China
基金
中国博士后科学基金; 美国国家科学基金会; 高等学校博士学科点专项科研基金;
关键词
MESOPOROUS SILICA SBA-15; PI-COMPLEXATION; ORGANOSULFUR COMPOUNDS; ADSORPTIVE DESULFURIZATION; TRANSPORTATION FUELS; POROUS MATERIALS; CO OXIDATION; DIESEL FUELS; Y ZEOLITES; REMOVAL;
D O I
10.1039/c2jm33216g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Deep desulfurization via pi-complexation adsorption is an effective method for the selective capture of thiophenic sulfur compounds. The adsorptive desulfurization capacity of an adsorbent has been demonstrated to strongly depend on the dispersion degree of active species. In the present study, a strategy was developed to promote the dispersion of copper species by directly using as-synthesized mesoporous silica SBA-15 as a support. The results show that the confined space between template and silica walls is highly efficient in dispersing the resultant guest oxide, and unusual CuO dispersion is realized. However, severe CuO aggregation occurs on the material prepared through the conventional method based on template-free SBA-15. Interestingly, copper precursors have a significant effect on the dispersion degree of the oxide, which decreases in the order nitrate > acetate > chloride. After autoreduction, the materials are active in adsorptive desulfurization, and the desulfurization performance relates well to the dispersion degree of the oxide. The present strategy allows template removal and precursor conversion in one step, avoids the repeated calcination in the conventional modification process, and saves time and energy. This strategy may open up an avenue for the design and synthesis of new functional materials by use of some particular micro environments.
引用
收藏
页码:18514 / 18521
页数:8
相关论文
共 51 条
[1]   NiWO4 nanoparticles: a promising catalyst for hydrodesulfurization [J].
Bi, Yunfei ;
Nie, Hong ;
Li, Dadong ;
Zeng, Shuangqin ;
Yang, Qinghe ;
Li, Mingfeng .
CHEMICAL COMMUNICATIONS, 2010, 46 (39) :7430-7432
[2]   Facile Synthesis of Ordered Mesoporous Alumina and Alumina-Supported Metal Oxides with Tailored Adsorption and Framework Properties [J].
Cai, Weiquan ;
Yu, Jiaguo ;
Anand, Chokkalingam ;
Vinu, Ajayan ;
Jaroniec, Mietek .
CHEMISTRY OF MATERIALS, 2011, 23 (05) :1147-1157
[3]   Preparation of Cu/SBA-15 catalysts by different methods for the hydrogenolysis of dimethyl maleate to 1,4-butanediol [J].
Chen, Liang-Feng ;
Guo, Ping-Jun ;
Zhu, Ling-Jun ;
Qiao, Ming-Hua ;
Shen, Wei ;
Xu, Hua-Long ;
Fan, Kang-Nian .
APPLIED CATALYSIS A-GENERAL, 2009, 356 (02) :129-136
[4]   Liquid phase adsorption by microporous coordination polymers: Removal of organosulfur compounds [J].
Cychosz, Katie A. ;
Wong-Foy, Antek G. ;
Matzger, Adam J. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (22) :6938-+
[5]   Enabling Cleaner Fuels: Desulfurization by Adsorption to Microporous Coordination Polymers [J].
Cychosz, Katie A. ;
Wong-Foy, Antek G. ;
Matzger, Adam J. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (40) :14538-14543
[6]   Thiophene capture with complex adsorbent SBA-15/Cu(I) [J].
Dai, Wei ;
Zhou, Yaping ;
Li, Shengnan ;
Li, Wu ;
Su, Wei ;
Sun, Yan ;
Zhou, Li .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2006, 45 (23) :7892-7896
[7]   Ordered porous materials for emerging applications [J].
Davis, ME .
NATURE, 2002, 417 (6891) :813-821
[8]   Extraordinarily High Activity in the Hydrodesulfurization of 4,6-Dimethyldibenzothiophene over Pd Supported on Mesoporous Zeolite Y [J].
Fu, Wenqian ;
Zhang, Lei ;
Tang, Tiandi ;
Ke, Qingping ;
Wang, Shun ;
Hu, Jianbo ;
Fang, Guoyong ;
Li, Jixue ;
Xiao, Feng-Shou .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (39) :15346-15349
[9]   Exploring in Situ Functionalization Strategy in a Hard Template Process: Preparation of Sodium-Modified Mesoporous Tetragonal Zirconia with Superbasicity [J].
Gong, Lu ;
Sun, Lin-Bing ;
Sun, Yuan-He ;
Li, Tian-Tian ;
Liu, Xiao-Qin .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (23) :11633-11640
[10]   Adjusting Host Properties to Promote Cuprous Chloride Dispersion and Adsorptive Desulfurization Sites Formation on SBA-15 [J].
He, Gu-Se ;
Sun, Lin-Bing ;
Song, Xue-Lin ;
Liu, Xiao-Qin ;
Yin, Yu ;
Wang, Yu-Chao .
ENERGY & FUELS, 2011, 25 (08) :3506-3513