Thermal stability and hydrogen release kinetics of ammonia borane under vehicle storage conditions

FUEL 102

Scot D. Rassat, sd.rassat@pnl.gov1, R. Scott Smith, zorro@pnl.gov2, Christopher L. Aardahl, christopher.aardahl@pnl.gov, Tom Autrey, Tom.Autrey@pnl.gov3, Arthur A. Chin, AChin@rohmhaas.com4, Joseph W. Magee4, Gary R. VanSciver4, and Frank J. Lipiecki4. (1) Environmental Technology Directorate, Pacific Northwest National Laboratory, P.O. Box 999, MS K6-28, Richland, WA 99352, (2) Fundamental Science Division, Pacific Northwest Laboratory, Richland, WA 99352, (3) Fundamental Science Division, Pacific Northwest National Laboratory, POB 999, MS#K2-57, Richland, WA 99352, (4) Rohm and Haas Company, Spring House, PA 19477-0904
Ammonia borane (AB) is a promising hydrogen storage material for fuel-cell vehicle applications owing to its high hydrogen density and stability under typical ambient conditions. The Department of Energy has defined technical targets for on-board storage systems including operating ambient temperatures up to 60°C. The thermal stability of solid AB from 40 to 60°C is investigated experimentally and computationally. Isothermal differential scanning calorimetry results from 70 to 90°C, in which hydrogen is released thermolytically and exothermically (deltaH ~ -22 kJ/mol), are characterized by modified Avrami kinetics, and the derived rate constants are fit to an Arrhenius expression (Ea ~160 kJ/mol). The results are used to project hydrogen release as a function of temperature, time, and initial AB conversion during isothermal and adiabatic storage. These calculations are compared to data obtained in the ARC® (Accelerated Rate Calorimeter), which is used to determine if the reaction is self-propagating under adiabatic storage conditions.