Base metal catalyzed dehydrogenation of ammonia-borane for chemical hydrogen storage

被引:587
作者
Keaton, Richard J. [1 ]
Blacquiere, Johanna M. [1 ]
Baker, R. Tom [1 ]
机构
[1] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
关键词
D O I
10.1021/ja066860i
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report here the first example of a homogeneous first row transition-metal-based catalyst which is active for dehydrogenation of ammonia-borane, H3NBH3, a promising chemical hydrogen storage material. Addition of ammonia-borane to an active catalyst formed in situ from the reaction of Ni(cod)(2) and 2 equiv of an appropriate N-heterocyclic carbene (NHC) rapidly evolves hydrogen at 60 degrees C. Using a gas burette to quantify the gas evolved, 29 of a possible 31 mL of H-2 for 3 equiv of H-2 was produced, equating to > 2.5 equiv of H-2 from ammonia-borane. Kinetic isotope effects of deuterated derivatives of ammonia-borane suggest that both N-H and B-H bonds are being broken in the rate-determining step(s).
引用
收藏
页码:1844 / +
页数:3
相关论文
共 18 条
[1]   LOW-COORDINATE CARBENE COMPLEXES OF NICKEL(0) AND PLATINUM(0) [J].
ARDUENGO, AJ ;
GAMPER, SF ;
CALABRESE, JC ;
DAVIDSON, F .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (10) :4391-4394
[2]   Thermal decomposition of B-N-H compounds investigated by using combined thermoanalytical methods [J].
Baitalow, F ;
Baumann, J ;
Wolf, G ;
Jaenicke-Rössler, K ;
Leitner, G .
THERMOCHIMICA ACTA, 2002, 391 (1-2) :159-168
[3]   BORYLIRIDIUM AND BORAETHYLIRIDIUM COMPLEXES FAC-[IRH2(PME3)3(BRR')] AND FAC-[IRH(PME3)3(ETA-2-CH2BHRR')] [J].
BAKER, RT ;
OVENALL, DW ;
CALABRESE, JC ;
WESTCOTT, SA ;
TAYLOR, NJ ;
WILLIAMS, ID ;
MARDER, TB .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1990, 112 (25) :9399-9400
[4]   Amineborane-based chemical hydrogen storage: Enhanced ammonia borane dehydrogenation in ionic liquids [J].
Bluhm, Martin E. ;
Bradley, Mark G. ;
Butterick, Robert, III ;
Kusari, Upal ;
Sneddon, Larry G. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (24) :7748-7749
[5]   In situ XAFS and NMR study of rhodium-catalyzed dehydrogenation of dimethylamine borane [J].
Chen, YS ;
Fulton, JL ;
Linehan, JC ;
Autrey, T .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (10) :3254-3255
[6]   Homogeneous, titanocene-catalyzed dehydrocoupling of amine-borane adducts [J].
Clark, Timothy J. ;
Russell, Christopher A. ;
Manners, Ian .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (30) :9582-9583
[7]   σ-Borane coordinated to nickel(0) and some related nickel(II) trihydride complexes [J].
Crestani, MG ;
Muñoz-Hernández, M ;
Arévalo, A ;
Acosta-Ramírez, A ;
García, JJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (51) :18066-18073
[8]   Efficient catalysis of ammonia borane dehydrogenation [J].
Denney, Melanie C. ;
Pons, Vincent ;
Hebden, Travis J. ;
Heinekey, D. Michael ;
Goldberg, Karen I. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (37) :12048-12049
[9]  
Dresselhaus M., 2003, BASIC ENERGY NEEDS H
[10]   PREPARATION, STRUCTURE, AND REACTIVITY OF 1,3,4-TRIPHENYL-4,5-DIHYDRO-1H-1,2,4-TRIAZOL-5-YLIDENE, A NEW STABLE CARBENE [J].
ENDERS, D ;
BREUER, K ;
RAABE, G ;
RUNSINK, J ;
TELES, JH ;
MELDER, JP ;
EBEL, K ;
BRODE, S .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1995, 34 (09) :1021-1023