hydrogen storage; metal borocarbides; metal fullerides; metal borides; first-principles electronic structure calculations; graphite; fullerene; graphene; intercalation compounds
Caputo Riccarda, Kupczak Arkadiusz, Sikora Wieslawa, Tekin Adem (2013), Ab initio crystal structure prediction by combining symmetry analysis representations and total energy calculations. An insight into the structure of Mg(BH4)(2), in PHYSICAL CHEMISTRY CHEMICAL PHYSICS
, 15(5), 1471-1480.
Caputo Riccarda (2013), Exploring the structure-composition phase space of lithium borocarbide, LixBC for x ≤ 1, in RSC ADVANCES
, 3(26), 10230-10241.
Pontiroli Daniele, Aramini Matteo, Gaboardi Mattia, Mazzani Marcello, Gorreri Alessandra, Ricco Mauro, Margiolaki Irene, Sheptyakov Denis (2013), Ionic conductivity in the Mg intercalated fullerene polymer Mg2C60, in CARBON
, 51, 143-147.
Caputo Riccarda, Tekin Adem (2012), Lithium Dihydroborate: First-Principles Structure Prediction of LiBH2, in INORGANIC CHEMISTRY
, 51(18), 9757-9765.
Mauron Philippe, Remhof Arndt, Bliersbach Andreas, Züttel Andreas, Sheptyakov Denis, Gaboardi Mattia, Choucair Mohammad, Pontiroli Daniele, Aramini Matteo, Ricco Mauro (2012), Reversible hydrogen absorption in sodium intercalated fullerenes, in INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
, 37(9), 14307-14314.
Kausteklis J, Cevc P, Arcon D, Nasi L, Pontiroli D, Mazzani M, Ricco M (2011), Electron paramagnetic resonance study of nanostructured graphite, in PHYSICAL REVIEW B
, 84(12), 1-5.
Ricco M, Pontiroli D, Mazzani M, Choucair M, Stride JA, Yazyev OV (2011), Muons Probe Strong Hydrogen Interactions with Defective Graphene, in NANO LETTERS
, 11(11), 4919-4922.
Ihara Y, Alloul H, Wzietek P, Pontiroli D, Mazzani M, Ricco M (2011), Spin dynamics at the Mott transition and in the metallic state of the Cs3C60 superconducting phases, in EPL
, 94(3), 1-6.
Mauron Philippe, Gaboardi Mattia, Remhof Arndt, Bliersbach Andreas, Sheptyakov Denis, Aramini Matteo, Vlahopoulou Gina, Giglio Fabio, Pontiroli Daniele, Riccò Mauro, Züttel Andreas, Hydrogen Sorption in Li12C60, in The Journal of Physical Chemistry C
Aramini Matteo, Gaboardi Mattia, Vlahopoulou Gina, Pontiroli Daniele, Cavallari Chiara, Milanese Chiara, Riccò Mauro, Muon spin relaxation reveals the hydrogen storage mechanism in light alkali metal fullerides, in Carbon
A key factor to enable the success of the hydrogen as a future fuel and hence to boost the hydrogen economy, is the development of active hydrogen storage systems. Current available technologies for on-board hydrogen storage (physical storage via compression and liquefaction, chemical storage in irreversible hydrogen carriers, reversible metal hydrides gas-on-solid adsorption) reveal inadequate and/or inefficient for a broader range of applications. Although it is clear that a compact, light, safe and affordable containment of hydrogen can only be achieved by adopting a solid absorber, the improvement of the solid state hydrogen storage capacity of the several materials proposed as good candidates, e.g. mixed metal hydrides, light metal borohydrides or alanates, still remain a central challenge. This in particular if referred to operative (p,T) conditions at which hydrogen can be desorbed and absorbed. Therefore, considerations of performance, cost, safety and geometric limitations have pushed the research in the direction to search for di fferent and improved solid state hydrogen storage materials. In the present project, we propose to investigate the possibility. to increase the hydrogen storage capacity of carbon-based materials via chemical activation by means of alkali and alkaline earth metal intercalation. The classes of materials we propose to investigate present two distinct molecular geometries: 1. planar carbon structures: boron-substituted graphite (BC)n and intercalated boron-substituted graphite, M(BC)n, M = Li;Mg; Ca; 2. close carbon structures: intercalated fullerene MxC60;M = Li; Na;Mg and light metal covered fullerene. Part of these materials has never been previously synthesized and none of them has been properly investigated with reference to their hydrogen storage capabilities. The central idea of our project is to take advantage of the electronic property modifications induced by heteroatom substitution, intercalation and coverage of graphite- and fullerene-like structures, to see whether hydrogen absorption is improved. In addition, the comparison between the two molecular arrangements, planar and close, will enable to highlight the key role of the molecular curvature on the absorption properties. For example, boron acts as electron acceptor and therefore can heavily modify the electronic properties of the host substrate, as in boro-substituted graphite layers. The expected contribution from each partner is therefore focused on giving answers to targeted questions in a joint and coordinated manner. The methodology, we will adopt, can be divided in two main highly interconnected parts. The first is focused on the synthesis and characterization of materials (substrates) to be hydrogenated and the second on the corresponding hydrogenated phase. The knowledge of phase stability, electronic and dynamic properties of the substrates is crucial to the subsequent hydrogenation and de-hydrogenation processes they will undergo. Accordingly, the core tasks, on which the cooperative and interdisciplinary approach is based, are: 1. theoretical and computational chemistry to model structures and derive those observables directly comparable with experimentally measurable quantities; 2. synthesis of the materials for hydrogen storage; 3. structural and chemico-physical property characterization of bare substrates and the corresponding hydrogenated phases; 4. hydrogenation processes, thermodynamics and kinetics of hydrogen absorption, to elucidate the mechanism of hydrogen sorption.