Tunable thermodynamics and kinetics for hydrogen storage : nanoparticle synthesis using ordered polymertemplates.

Conference · Thu Apr 01 04:00:00 EDT 2010

OSTI ID:1003964

Allendorf, Mark D

Theory and experiment suggest nanoscale hydride particles are destabilized relative to bulk, but the origin of this effect is unclear. Both size and local environment may play a role. The overall project objective is to achieve tunable thermodynamics for hydrogen storage materials by controlling nanoparticle size, composition, and environment. Key Goals for FY09 are: (1) Demonstrate and downselect infiltration methods; (2) Measure desorption kinetics for MgH{sub 2} and NaAlH{sub 4} nanoparticles and LiBH{sub 4} thin films; (3) Benchmark DFT and atomistic nanoparticle models using Quantum Monte Carlo (QMC); and (4) Quantify effect of nanoparticle size on {Delta}H{sub d}{sup o} using MgH{sub 2} as initial example. Summary of the key results are: (1) New highly ordered nanoporous templates enable systematic probing of nanoscale effects - Nanoscale NaAlH{sub 4} particles (as small as 1.5 nm diameter) exhibit improved H{sub 2} desorption kinetics relative to bulk and Preliminary data suggest MgH{sub 2} nanoparticle formation and possibly improved desorption kinetics; (2) Benchmarking DFT against QMC reveals significant errors that are non-systematic (H{sub 2} desorption energies underpredicted by as much as 30 kJ/mol); (3) QMC predicts greatest effect of size is for extremely small particles; e.g. (MgH{sub 2}){sub n}, n {le} 6 which is much smaller than predicted by Wolfe construction approach and observed in experiments and it suggests factors other than electronic structure (e.g. surrounding chemical environment) influence stability; (4) New NanoPEGS code developed and tested for MgH{sub 2} 2particles; and (5) New mass spec tool (STMBMS) reveals key details of hydrogen desorption process.

• Research Organization: Sandia National Laboratories
• Sponsoring Organization: USDOE
• DOE Contract Number: AC04-94AL85000
• OSTI ID: 1003964
• Report Number(s): SAND2010-2419C
• Country of Publication: United States
• Language: English

Related Subjects

08 HYDROGEN
BENCHMARKS
CONSTRUCTION
DESORPTION
ELECTRONIC STRUCTURE
HYDRIDES
HYDROGEN
HYDROGEN STORAGE
KINETICS
ORIGIN
POLYMERS
STABILITY
SYNTHESIS
THERMODYNAMICS
THIN FILMS