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We report on hydrogen adsorption and desorption on titanium-covered graphene in order to test theoretical proposals to use of graphene functionalized with metal atoms for hydrogen storage. At room temperature titanium islands grow with an average diameter of about 10 nm. Samples were then loaded with hydrogen, and its desorption kinetics was studied by thermal desorption spectroscopy. We observe the desorption of hydrogen in the temperature range between 400K and 700 K. Our results demonstrate the stability of hydrogen binding at room temperature and show that hydrogen desorbs at moderate temperatures in line with what required for practical hydrogen-storage applications.
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The ability of atomic hydrogen to chemisorb on graphene makes the latter a promising material for hydrogen storage. Based on scanning tunneling microscopy techniques, we report on site-selective adsorption of atomic hydrogen on convexly curved regions of monolayer graphene grown on SiC(0001). This system exhibits an intrinsic curvature owing to the interaction with the substrate. We show that at low coverage hydrogen is found on convex areas of the graphene lattice. No hydrogen is detected on concave regions. These findings are in agreement with theoretical models which suggest that both binding energy and adsorption barrier can be tuned by controlling the local curvature of the graphene lattice. This curvature-dependence combined with the known graphene flexibility may be exploited for storage and controlled release of hydrogen at room temperature making it a valuable candidate for the implementation of hydrogen-storage devices.
Hydrogen adsorption on graphene-supported metal clusters has brought much controversy due to the complex nature of the bonding between hydrogen and metal clusters. The bond types of hydrogen and graphene-supported Ti clusters are experimentally and theoretically investigated. Transmission electron microscopy shows that Ti clusters of nanometer-size are formed on graphene. Thermal desorption spectroscopy captures three hydrogen desorption peaks from hydrogenated graphene-supported Ti clusters. First principle calculations also found three types of interaction: Two types of bonds with different partial ionic character and physisorption. The physical origin for this rests on the charge state of the Ti clusters: when Ti clusters are neutral, H2 is dissociated, and H forms bonds with the Ti cluster. On the other hand, H2 is adsorbed in molecular form on positively charged Ti clusters, resulting in physisorption. Thus, this work clarifies the bonding mechanisms of hydrogen on graphene-supported Ti clusters.
The graphene-enhanced Raman scattering of Rhodamine 6G molecules on pristine, fluorinated and 4-nitrophenyl functionalized graphene substrates was studied. The uniformity of the Raman signal enhancement was studied by making large Raman maps. The relative enhancement of the Raman signal is demonstrated to be dependent on the functional groups, which was rationalized by the different doping levels of pristine, fluorinated and 4-nitrophenyl functionalized graphene substrates. The impact of the Fermi energy of graphene and the phonon energy of the molecules was considered together for the first time in order to explain the enhancement. Such approach enables to understand the enhancement without assuming anything about the uniformity of the molecules on the graphene surface. The agreement between the theory and our measured data was further demonstrated by varying excitation energy.
Titanium-island formation on graphene as a function of defect density is investigated. When depositing titanium on pristine graphene, titanium atoms cluster and form islands with an average diameter of about 10nm and an average height of a few atomic layers. We show that if defects are introduced in the graphene by ion bombardment, the mobility of the deposited titanium atoms is reduced and the average diameter of the islands decreases to 5nm with monoatomic height. This results in an optimized coverage for hydrogen storage applications since the actual titanium surface available per unit graphene area is significantly increased.
We report on heat conduction properties of thermal interface materials with self-aligning magnetic grapheme fillers. Graphene enhanced nano-composites were synthesized by an inexpensive and scalable technique based on liquid-phase exfoliation. Functionalization of graphene and few-layer-graphene flakes with Fe3O4 nanoparticles allowed us to align the fillers in an external magnetic field during dispersion of the thermal paste to the connecting surfaces. The filler alignment results in a strong increase of the apparent thermal conductivity and thermal diffusivity through the layer of nano-composite inserted between two metallic surfaces. The self-aligning magnetic grapheme fillers improve heat conduction in composites with both curing and non-curing matrix materials. The thermal conductivity enhancement with the oriented fillers is a factor of two larger than that with the random fillers even at the low ~1 wt. % of graphene loading. The real-life testing with computer chips demonstrated the temperature rise decrease by as much as 10oC with use of the non-curing thermal interface material with ~1 wt. % of the oriented fillers. Our proof-of-concept experiments suggest that the thermal interface materials with functionalized graphene and few-layer-graphene fillers, which can be oriented during the composite application to the surfaces, can lead to a new method of thermal management of advanced electronics.
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