Publications

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This research and development project is focused on the advancement of a technology that produces hydrogen at a cost that is competitive with fossil-based fuels for transportation. A twostep, solar-driven WS thermochemical cycle is theoretically capable of achieving an STH conversion ratio that exceeds the DOE target of 26% at a scale large enough to support an industrialized economy [1]. The challenge is to transition this technology from the laboratory to the marketplace and produce hydrogen at a cost that meets or exceeds DOE targets.

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In this paper, we offer a perspective on the current state of material research in a part of the solar fuels community that exploits process heat derived from concentrated solar energy to power simple thermochemical gas-splitting cycles. The working fluid in this process is a nonstoichiometric oxide subject to extreme conditions that repeatedly distorts the lattice by forcing oxygen atoms to move in and out of the crystal. This technology is currently challenged by a need to discover optimal materials and derive robust processes to increase cycle efficiency. In the realm of emerging technologies for converting solar insulation to portable and storable energy carriers, this approach has already proven to be scalable with demonstrations that approach 100 kW. Innovations in materials and methods are required to increase solar utilization and process efficiency in order to achieve commercial viability.

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Recent work regarding the efficiency maximization for solar thermochemical fuel production in two step cycles has led to the design of a new type of reactor—the cascading pressure reactor—in which the thermal reduction step of the cycle is completed in multiple stages, at successively lower pressures. This approach enables lower thermal reduction pressures than in single-staged reactors, and decreases required pump work, leading to increased solar to fuel efficiencies. In this work we report on the design and construction of a prototype cascading pressure reactor and testing of some of the key components. We specifically focus on the technical challenges particular to the design, and their solutions.

Recent work regarding the efficiency maximization for solar thermochemical fuel production in two step cycles has led to the design of a new type of reactor - the cascading pressure reactor - in which the thermal reduction step of the cycle is completed in multiple stages, at successively lower pressures. This approach enables lower thermal reduction pressures than in single-staged reactors, and decreases required pump work, leading to increased solar to fuel efficiencies. Here we report on the design and construction of a prototype cascading pressure reactor and testing of some of the key components. We especially focus on the technical challenges particular to the design, and their solutions.

Preparation of sodium zirconium silicate phosphate (NaSICon), Na_1+xZr₂Si_xP_3–xO₁₂ (0.25 ≤ x ≤ 1.0), thin films has been investigated via a chemical solution approach on platinized silicon substrates. Increasing the silicon content resulted in a reduction in the crystallite size and a reduction in the measured ionic conductivity. Processing temperature was also found to affect microstructure and ionic conductivity with higher processing temperatures resulting in larger crystallite sizes and higher ionic conductivities. The highest room temperature sodium ion conductivity was measured for an x = 0.25 composition at 2.3 × 10^–5 S/cm. In conclusion, the decreasing ionic conductivity trends with increasing silicon content and decreasing processing temperature are consistent with grain boundary and defect scattering of conducting ions.

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Next generation metal-ion conducting membranes are key to developing energy storage and utilization technologies like batteries and fuel ce lls. Sodium super-ionic conductors (aka NaSICON) are a class of compounds with AM 1 M 2 (PO 4 ) 3 stoichiometry where the choice of "A" and "M" cation varies widely. This report, which de scribes substitutional derivatives of NZP (NaZr 2 P 3 O 12 ), summarizes the accomplishments of a Laboratory D irected Research and Development (LDRD) project to analyze transport mec hanisms using a combination of in situ studies of structure, composition, and bonding, com bined with first principles theory and modeling. We developed an experimental platform and applied methods, such as synchrotron- based X-ray spectroscopies, to probe the electronic structure of compositionally well-controlled NaSICON films while in operation ( i.e ., conducting Na ions exposed to oxygen or water va por atmospheres). First principles theory and modeling were used to interpret the experimental observations and develop an enhanced understanding of atomistic processes that give rise to, and affect, ion conduction.

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