Zeolite confined rhodium(0) nanoclusters as highly active, reusable, and long-lived catalyst in the methanolysis of ammonia-borane

被引:88
作者
Caliskan, Salim [1 ]
Zahmakiran, Mehmet [1 ]
Ozkar, Saim [1 ]
机构
[1] Middle E Tech Univ, Dept Chem, TR-06531 Ankara, Turkey
关键词
Rhodium; Nanocluster; Zeolite; Methanolysis; Catalysis; Ammonia-borane; HYDROGEN GENERATION; RUTHENIUM(0) NANOCLUSTERS; THERMAL-DECOMPOSITION; FAUJASITE ZEOLITES; HYDROLYSIS; STORAGE; NANOPARTICLES; DEHYDROGENATION; DISSOCIATION; REUSABILITY;
D O I
10.1016/j.apcatb.2009.10.013
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
Addressed herein is the preparation, characterization and the catalytic use of zeolite confined rhodium(0) nanoclusters in the methanolysis of ammonia-borane. Rhodium(0) nanoclusters; could be generated in zeolite-Y by a two-step procedure: (i) incorporation of rhodium(Ill) cations into the zeolite-Y by ion-exchange and (ii) reduction of rhodium(Ill) ions within the zeolite cages by sodium borohydride in aqueous solution, followed by filtration and dehydration by heating to 550 degrees C under 10(-4) Torr. Zeolite confined rhodium(0) nanoclusters are stable enough to be isolated as solid materials and characterized by ICP-OES, XRD. SEM, EDX, HR-TEM, XPS and N-2 adsorption-desorption technique. The zeolite confined rhodium(0) nanoclusters are isolable, bottleable, redispersible and reusable as an active catalyst in the methanolysis of ammonia-borane even at low temperatures. They provide exceptional catalytic activity with an average value of TOF = 380 h(-1) and unprecedented lifetime with 74,300 turnovers in the methanolysis of ammonia-borane at 25 +/- 0.1 degrees C. The work reported here also includes the full experimental details of the collection of a wealth of previously unavailable kinetic data to determine the rate law, and activation parameters (E-a, Delta H-not equal and Delta S-not equal) for the catalytic methanolysis of ammonia-borane. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:387 / 394
页数:8
相关论文
共 43 条
[1]  
[Anonymous], 2007, LIGHT WAY SUST EN FU
[2]  
[Anonymous], 2003, BAS EN SCI WORKSH HY
[3]   Hydrogen storage in high surface area carbon nanotubes produced by catalytic chemical vapor deposition [J].
Bacsa, R ;
Laurent, C ;
Morishima, R ;
Suzuki, H ;
Le Lay, M .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (34) :12718-12723
[4]   FREQUENCY AND INTENSITY CONSIDERATIONS IN THE FAR-INFRARED SPECTROSCOPY OF FAUJASITE ZEOLITES - EXPERIMENT AND THEORY - METAL CATION VIBRATIONAL ASSIGNMENTS, SITE LOCATIONS, AND POPULATIONS [J].
BAKER, MD ;
GODBER, J ;
OZIN, GA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1985, 107 (11) :3033-3043
[5]  
Breck D.W., 1984, Zeolite molecular sieves
[6]   Room temperature hydrogen generation from aqueous ammonia-borane using noble metal nano-clusters as highly active catalysts [J].
Chandra, Manish ;
Xu, Qiang .
JOURNAL OF POWER SOURCES, 2007, 168 (01) :135-142
[7]   Dissociation and hydrolysis of ammonia-borane with solid acids and carbon dioxide: An efficient hydrogen generation system [J].
Chandra, Manish ;
Xu, Qiang .
JOURNAL OF POWER SOURCES, 2006, 159 (02) :855-860
[8]   A high-performance hydrogen generation system: Transition metal-catalyzed dissociation and hydrolysis of ammonia-borane [J].
Chandra, Manish ;
Xu, Qiang .
JOURNAL OF POWER SOURCES, 2006, 156 (02) :190-194
[9]   Interaction of hydrogen with metal nitrides and imides [J].
Chen, P ;
Xiong, ZT ;
Luo, JZ ;
Lin, JY ;
Tan, KL .
NATURE, 2002, 420 (6913) :302-304
[10]   Ni1-xPtx (x=0-0.12) hollow spheres as catalysts for hydrogen generation from ammonia borane [J].
Cheng, Fangyi ;
Ma, Hua ;
Li, Yueming ;
Chen, Jun .
INORGANIC CHEMISTRY, 2007, 46 (03) :788-794