Nanoscaffold Mediates Hydrogen Release and the Reactivity of Ammonia Borane

Angewandte Chemie - International Edition - Tập 44 Số 23 - Trang 3578-3582 - 2005
Anna Gutowska1, Liyu Li1, Yongsoon Shin1, Chongmin M. Wang1, Xiaohong S. Li1, John C. Linehan1, R. Scott Smith1, Bruce D. Kay1, Benjamin Schmid2, Wendy J. Shaw1, Maciej Gutowski1, Tom Autrey1
1Pacific Northwest National Laboratory, Richland, WA 99352, USA, Fax: (+1) 509-375-6660
2University of Oregon, Department of Chemistry, Eugene, OR, USA

Tóm tắt

Từ khóa


Tài liệu tham khảo

10.1038/424129a

10.1038/35104599

L. de Palacio P. Busquin Report from Europa Commission “Hydrogen Energy and Fuels Cells: A Vision for Our Future” http://europa.eu.int/comm/research/energy/nn/nn_rt/nn_rt_hlg/article_1146_en.htm.

Recent information can be found at:http://www.eere.energy.gov/hydrogenandfuelcells/pdfs/freedomcar_targets_explanations.pdf.

10.1021/cr030691s

10.1016/S0925-8388(01)01662-0

10.1038/nature01210

10.1126/science.1083440

10.1038/35104634

10.1021/nl015576g

10.1038/386377a0

10.1016/S0925-8388(01)01586-9

10.1016/S0008-6223(01)00051-3

M.Gutowski T.Autrey J.Linehan unpublished results.

Pauling L., 1988, General Chemistry, 182

10.1021/ja01534a001

J. Baumann Dissertation Physikalisch‐chemische Untersuchungen zur Wasserstoffabgabe von BNH‐Verbindungen 2003 TU‐Bergakademie Freiberg Germany. The research group in Freiberg has been investigating NH3BH3as a hydrogen‐storage material.

10.1016/S0040-6031(02)00173-9

10.1016/0040-6031(87)88340-5

Gutowski M., 2004, Prepr. Pap. Am. Chem. Soc. Div. Fuel Chem., 49, 275

10.1016/S0040-6031(99)00365-2

Liang J., 2003, Prepr. Pap. Am. Chem. Soc. Div. Fuel Chem., 48, 281

10.1016/S0921-4526(02)01814-8

10.1002/3527607420.ch24

10.1016/S0925-8388(01)01645-0

10.1126/science.279.5350.548

10.1002/1521-3757(20000804)112:15<2814::AID-ANGE2814>3.0.CO;2-S

10.1002/1521-3773(20000804)39:15<2702::AID-ANIE2702>3.0.CO;2-F

The 800‐MHz solid‐state NMR spectrum is available as Supporting Information. Observed11B resonances: AB:SBA‐15 (one signal δ=−23 ppm) neat AB (four signals δ=−6 −12 −23 −37 ppm).

van 't Hoff equation: ln(peq/${p{{{\rm o}\hfill \atop {\rm eq}\hfill}}}$)=ΔH/RT−ΔS/R. The difference in hydrogen overpressure can be calculated from ΔΔHof H2loss from AB bulk and AB in the scaffold. Δln(peq/${p{{{\rm o}\hfill \atop {\rm eq}\hfill}}}$)=ΔΔH/RT−ΔΔS/R. ΔΔS=0 ΔΔH=20 kJ mol−1 thenpeq(AB)/peq(AB:SBA‐15)=4667. As ΔH≈0 in the scaffold the pressure required for H2uptake by the spent AB is the pressure required to overcome the entropy of formation of the gaseous H2. Reversibility processes will be addressed in a subsequent publication.

10.1021/ja994361u

10.1016/S0378-7753(03)00054-5

10.1021/ja974025i