The discovery of effective hydrogen storage materials is fundamental for the progress of a clean energy economy. Ammonia borane (H 3 BNH 3 , AB) has attracted great interest as a promising candidate but the reaction path that leads from its solid phase to hydrogen release is not yet fully understood. To address the need for insights in the atomistic details of such a complex solid state process, in this work we use ab-initio molecular dynamics and metadynamics to study the early stages of AB dehydrogenation. We show that the formation of ammonia diborane (H 3 NBH 2 (μ-H)BH 3 ) leads to the release of NH 4+ , which in turn triggers an autocatalytic H 2 production cycle. Our calculations provide a model for how complex solid state reactions can be theoretically investigated and rely upon the presence of multiple ammonia borane molecules, as substantiated by standard quantum-mechanical simulations on a cluster.

The Onset of Dehydrogenation in Solid Ammonia Borane: An Ab Initio Metadynamics Study

Sicilia, Emilia;Russo, Nino;PARRINELLO, Michele
2019

Abstract

The discovery of effective hydrogen storage materials is fundamental for the progress of a clean energy economy. Ammonia borane (H 3 BNH 3 , AB) has attracted great interest as a promising candidate but the reaction path that leads from its solid phase to hydrogen release is not yet fully understood. To address the need for insights in the atomistic details of such a complex solid state process, in this work we use ab-initio molecular dynamics and metadynamics to study the early stages of AB dehydrogenation. We show that the formation of ammonia diborane (H 3 NBH 2 (μ-H)BH 3 ) leads to the release of NH 4+ , which in turn triggers an autocatalytic H 2 production cycle. Our calculations provide a model for how complex solid state reactions can be theoretically investigated and rely upon the presence of multiple ammonia borane molecules, as substantiated by standard quantum-mechanical simulations on a cluster.
ammonia borane; computational chemistry; dehydrogenation; quantum chemistry; reaction mechanisms; Catalysis; Chemistry (all)
File in questo prodotto:
Non ci sono file associati a questo prodotto.

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11770/291240
 Attenzione

Attenzione! I dati visualizzati non sono stati sottoposti a validazione da parte dell'ateneo

Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 21
  • ???jsp.display-item.citation.isi??? 27
social impact