Marie Curie Fellowship Enables Lueking's study at the University of Crete

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Professor Angela Lueking has been awarded a highly competitive Marie Curie International Incoming Fellowship to partner with researchers at the University of Crete to study basics of hydrogen adsorption and diffusion on surfaces.  The work will include design of novel materials.  The abstract for the successful proposal is included below.

Objectives and Overview:  The objective of the proposed work is to synthesize catalyzed nanoporous materials that have superior hydrogen uptake between 300K and 400K and moderate pressures (20-100 bar) via the hydrogen spillover mechanism. Hydrogen spillover involves addition of a catalyst to a high-surface area microporous support, such that the catalyst acts as a source for atomic hydrogen, the atomic hydrogen diffuses from the catalyst to the support, and ideally, the support provides a high number of tailored surface binding sites to maximize the number of atomic hydrogens interacting with the surface.  The proposed work will provide a means to explore an extended collaboration to combine in situ spectroscopic techniques and theoretical multi-scale modelling calculations. Both carbon-based and microporous metal-organic framework (MMOF) materials with added hydrogen dissociated catalysts will be drawn from past and on-going projects, in order to identify specific binding sites that lead to appreciable uptake.  First, preliminary spectroscopic data will be used to validate and extend existing theoretical models. In situ characterization of materials with systematic variations in structure and/or synthesis will be used to identify properties that lead to high uptake, including effect of structure, geometry, surface chemistry, and catalyst-support interface. Resulting spectroscopic data will be analyzed with theoretical models to conclusively identify the nature of the binding site. Validated models will be used to direct future synthesis of novel materials.  The overall goal will be to identify tailored surface sites that reversibly bind atomic hydrogen between 300 K and 400K.

The work is incredibly timely, as the hydrogen spillover mechanism has become highly controversial in the past two years, due largely to discrepancies between laboratories, and even variations of the magnitude of uptake observed for materials prepared with near-identical techniques within the same laboratory. Amidst this controversy, a combined approach of in situ spectroscopic techniques and theoretical multi-scale modelling calculations will resolve the hydrogen spillover mechanism and illuminate the nature of the exact surface sites and structure responsible for the high uptake in select materials. The proposed work extends previous work of Professor Angela Lueking, who as a graduate student, was first author on the first papers identifying hydrogen spillover as a means to achieve appreciable uptake at room temperature. Subsequently, Lueking has studied hydrogen uptake and adsorption in other materials, and furthered her experience in material characterization. She has recently returned to the field of hydrogen spillover, employing in situ spectroscopic techniques,5, 6 as outlined below.  Lueking will pair with George Froudakis of the University of Crete, whose theoretical calculations (with George Psofogiannakis, a current Marie Curie fellow) provided the first multi-scale modelling of the hydrogen spillover mechanism. The proposed work will provide a means to explore an extended collaboration to combine their respective work in experiment and theory.  The combined approach is expected to not only resolve what has become a highly controversial issue in the literature, but ultimately, identification of the key sites responsible for high uptake in select materials is expected to lead to a significant increase in capacity and reproducibility in hydrogen spillover materials that are optimized for near-ambient temperature adsorption.


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