Lithium-ion batteries (LIBs) are ubiquitous in everyday applications. However, Lithium (Li) is a limited resource on the planet and, therefore, not sustainable. As an alternative to lithium, earth-abundant and cheaper multivalent metals such as aluminum (Al) and calcium (Ca) have been actively researched in battery systems. However, finding suitable intercalation hosts for multivalent-ion batteries is urgently needed. Open-tunneled oxides represent a specific category of microparticles distinguished by the presence of integrated one-dimensional channels or nanopores. This work focuses on two promising open-tunnel oxides: Niobium Tungsten Oxide (NTO) and Molybdenum Vanadium Oxide (MoVO). The MoVO structure can accommodate a larger number of multivalent ions than NTO due to its larger surface area and different shapes. Specifically, the MoVO structure can adsorb Ca, Li, and Al ions with adsorption potentials ranging from around 4 to 5 eV. However, the adsorption potential for hexagonal channels of Al ion drops to 1.73 eV due to the limited channel area. The NTO structure exhibits an insertion/adsorption potential of 4.4 eV, 3.4 eV, and 0.9 eV for one Li, Ca, and Al, respectively. Generally, Ca ions are more readily adsorbed than Al ions in both MoVO and NTO structures. Bader charge analysis and charge density plots reveal the role of charge transfer and ion size in the insertion of multivalent ions such as Ca and Al into MoVO and NTO systems. Exploring open-tunnel oxide materials for battery applications is hindered by vast compositional possibilities. The execution of experimental trials and quantum-based simulations is not viable for addressing the challenge of locating a specific item within a large and complex set of possibilities. Therefore, it is imperative to conduct structural stability testing to identify viable combinations with sufficient pore topologies. Data mining and machine learning techniques are employed to discover innovative transitional metal oxide materials. This study compares two machine learning algorithms, one utilizing descriptors and the other employing graphs to predict the synthesizability of new materials inside a laboratory setting. The outcomes of this study offer valuable insights into the exploration of alternative naturally occurring multiscale particles.
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In Situ Studies of the Formation of Tungsten and Niobium Oxide Nanoparticles: Towards Automated Analysis of Reaction Pathways from PDF Analysis using the Pearson Correlation Coefficient
Using Pair Distribution Function (PDF) analysis of in situ total scattering data, we investigate the formation of tungsten and niobium oxides in a simple solvothermal synthesis. We use Pearson Correlation Coefficient (PCC) analysis of the time resolved PDFs to both map the structural changes taking place throughout the synthesis and identify structural models for precursor and product through PCC‐based structure mining. Our analysis first shows that ultra‐small tungsten and niobium oxide nanoparticles form instantaneously upon heating, with sizes between 1.5 and 2 nm. We show that the main structural motifs in the nanoparticles can be described with structures containing pentagonal columns, which is characteristic for many bulk tungsten and niobium oxides. We furthermore elucidate the structure of the precursor complex as clusters of octahedra with O‐ and Cl‐ligands. The PCC based methodology automates the structure characterization and proves useful for analysis of large datasets of for example, time resolved X‐ray scattering studies. The PCC is implemented in ‘PDF in the cloud’, a web platform for PDF analysis.
more » « less- Award ID(s):
- 1922234
- NSF-PAR ID:
- 10443944
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Chemistry–Methods
- Volume:
- 2
- Issue:
- 9
- ISSN:
- 2628-9725
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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