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The transition from fossil fuels to renewable energy requires the development of efficient and cost-effective energy storage technologies. A promising way forward is to harness the energy of intermittent renewable sources, such as solar and wind, to perform (electro)catalytic reactions to generate fuels, thus storing energy in the form of chemical bonds. Furthermore, current catalysts rely on the use of expensive, rare, or geographically localized elements, such as platinum. Widespread adoption of new (electro)catalytic technologies hinges on the discovery and development of materials containing earth-abundant elements, which can efficiently catalyze an array of (electro)chemical reactions.
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Many chemical processes depend on having an environment that is low in oxygen partial pressure (P O2 < 100 Pa); sorption pumps are a promising route to establishing that environment by either oxygen pumping or oxygen separation from an inert gas. Near ambient sorption-based processes rely on either pressure or thermal swings, requiring no moving parts, no electricity, and neither very high nor very low temperatures. In this work, we use ab initio calculations to explore zeolites as a class of materials for sorption based oxygen pumping/separation. Our calculations indicate that while the neat ALPO-5 zeolite does not adsorb O 2 , O 2 does adsorb on zeolites selectively substituted with transition metals and metalloids and hence, can enable separation and pumping. ALPO-5 substituted with Si, Ge, Sn, Pd, Pt, Ti, V, Cr, Mn, Zr, Mo, Hf, W, Ce, and Pr provides adsorption energies ranging from -0.19 to -3.92 eV, (-) indicates exothermic process. Additionally, we provide a comprehensive understanding of what controls the adsorption energy: 1) the substi-tutions must be able to adopt an oxidation state that is more positive than the cation it replaces, and 2) the size of the pore into which the O 2 adsorbs to the wall. Additionally, we conduct a ther-modynamic analysis of a thermal swing cycle to approximate the optimal O 2 binding energy for 2 low energy O 2 pumping/separation. We find that the minimum energy cost likely occurs when the adsorption energy is in the range of 0.75 – 1.00 eV (72 – 97 kJ·mol -1 ), which corresponds to Ge, V, Pt, or Ce substituted ALPO-5.
Photoelectrochemical performance dependence upon absorption length, carrier diffusion length, and surface area of an oxynitride photoabsorber is investigated. How best to fabricate optical-quality thin films of bandgap-tunable oxynitrides is also discussed. We targeted the stoichiometric compound SrNbO 2 N as an optimal wide-bandgap photoabsorber (1.9 eV) for use with silicon (1.1 eV) in a tandem structure photoelectrochemical cell. Preparation of perovskite oxynitrides at high-temperature as isolated powders is often straightforward, but it is difficult to integrate them as thin films in tandem junction devices with low-temperature materials. Here we develop the first method to prepare optical-quality SrNbO 2 N thin-films of tunable thickness and roughness on single-crystal silicon substrate. This achievement required an interfacial layer of ultra-thin TaN to be used as a barrier to reduce the inter-diffusion of silicon and oxygen during oxynitride syn-thesis. We produced a variety of SrNbO 2 N film thicknesses (20-440 nm) on n + -Si(100) surfaces. Roughness factor (0.14-21) scaled with thickness. The intrinsic photoelectrochemical activity of these devices was evaluated using a low-barrier sacrificial electron donor. Photocurrent density and photovoltage revealed a significant (and non-linear) dependence on film thickness and roughness. Furthermore, absorption length, carrier diffusion length, and surface area were each found to play key roles. Balancing these is required for optimally performing devices.
Closed, laser-induced optical transitions (“optical cycling transitions”) of molecules can be used for state preparation and measurement in quantum information science and quantum sensing. Increasingly complex molecular species supporting optical cycling can provide new capabilities for quantum science, and it is not clear if there is a limit on their size or complexity. We explore Ca–O–L molecular constructs to support the optical cycling center, Ca, with ligands, L, being arenes. We find that L can be as large as coronene (i.e., CaOC 24 H 11 ) without losing the diagonality of the Franck–Condon factor (FCF). Furthermore, L can be substituted with electron-withdrawing groups to improve the FCF. Larger L, beyond ~7 rings, can disrupt the diagonality of the FCF by closing the HOMO–LUMO ligand electronic state gap and reordering with the local states on the cycling center. Altogether, we find that optical cycling can be retained for arenes, and we offer a principle for their design.