2024 New's Items

Design Principles and Routes for Calcium Alkoxyaluminate Electrolytes

Leon, N. J.
Ilic, S.
Xie, X.
Jeong, H.
Yang, Z.
Wang, B.
Spotte-Smith, E. W. C.
Stern, C.
Hahn, N.
Zavadil, K.
Cheng, L.
Persson, K. A.
Connell, J. G.
Liao, C.
2024

Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. At present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA]2, where [TPFA]− = [Al(OC(CF3)3)4]− and Ca[B(hfip)4]2...

First-Principles and Experimental Investigation of ABO4 Zircons as Calcium Intercalation Cathodes

Kim, J.
Sari, D.
Chen, Q.
Rutt, A.
Ceder, G.
Persson, K. A.
2024

Identifying next-generation batteries with multivalent ions, such as Ca2+ is an active area of research to meet the increasing demand for large-scale, renewable energy storage solutions. Despite the promise of higher energy densities with multivalent batteries, one of their main challenges is addressing the sluggish kinetics in cathodes that arise from stronger electrostatic interactions between the multivalent ion and host lattice. In this paper, zircons are theoretically and experimentally evaluated as Ca cathodes. A migration barrier as low as 113 meV is...

Switching the spin cycloid in BiFeO3 with an electric field

Meisenheimer, P.
Moore, G.
Zhou, S.
Zhang, H.
Huang, X.
Husain, S.
Chen, X.
Martin, L. W.
Persson, K. A.
Griffin, S.
Caretta, L.
Stevenson, P.
Ramesh, R.
2024

Bismuth ferrite (BiFeO3) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO3 are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements. Using nitrogen vacancy-based diamond magnetometry, we observe the magnetic spin cycloid structure of...

Deconvolution and Analysis of the 1H NMR Spectra of Crude Reaction Mixtures

Venetos, M. C.
Elkin, M.
Delaney, C.
Hartwig, J. F.
Persson, K. A.
2024

Nuclear magnetic resonance (NMR) spectroscopy is an important analytical technique in synthetic organic chemistry, but its integration into high-throughput experimentation workflows has been limited by the necessity of manually analyzing the NMR spectra of new chemical entities. Current efforts to automate the analysis of NMR spectra rely on comparisons to databases of reported spectra for known compounds and, therefore, are incompatible with the exploration of new chemical space. By reframing the NMR spectrum of a reaction mixture as a joint probability distribution, we have used...

Oxygen Transport through Amorphous Cathode Coatings in Solid-State Batteries

Cheng, J.
Peng, X.
Zhang, Y.-Q.
Tian, Y.
Ogunfunmi, T.
Haddad, A. Z.
Dopilka, A.
Ceder, G.
Persson, K. A.
Scott, M. C.
2024
All solid-state batteries (SSBs) are considered the most promising path to enabling higher energy-density portable energy, while concurrently improving safety as compared to current liquid electrolyte solutions. However, the desire for high energy necessitates the choice of high-voltage cathodes, such as nickel-rich layered oxides, where degradation phenomena related to oxygen loss and structural densification at the cathode surface are known to significantly compromise the cycle and thermal stability. In this work, we show, for the first time, that even in an SSB, and when protected by...

Complete miscibility of immiscible elements at the nanometre scale

Chen, P.-C.
Gao, M.
McCandler, C. A.
Song, C.
Jin, J.
Yang, Y.
Maulana, A. L.
Persson, K. A.
Yang, P.
2024

Understanding the mixing behaviour of elements in a multielement material is important to control its structure and property. When the size of a multielement material is decreased to the nanoscale, the miscibility of elements in the nanomaterial often changes from its bulk counterpart. However, there is a lack of comprehensive and quantitative experimental insight into this process. Here we explored how the miscibility of Au and Rh evolves in nanoparticles of sizes varying from 4 to 1 nm and composition changing from 15% Au to 85% Au. We found that the two immiscible elements exhibit a...

Structured information extraction from scientific text with large language models

Dagdelen, J.
Dunn, A.
Lee, S.
Walker, N.
Rosen, A. S.
Ceder, G.
Persson, K. A.
Jain, A.
2024

Extracting structured knowledge from scientific text remains a challenging task for machine learning models. Here, we present a simple approach to joint named entity recognition and relation extraction and demonstrate how pretrained large language models (GPT-3, Llama-2) can be fine-tuned to extract useful records of complex scientific knowledge. We test three representative tasks in materials chemistry: linking dopants and host materials, cataloging metal-organic frameworks, and general composition/phase/morphology/application information extraction. Records are extracted from...

Mechanistically Guided Materials Chemistry: Synthesis of Ternary Nitrides, CaZrN2 and CaHfN2

Rom, C. L.
Novick, A.
McDermott, M. J.
Yakovenko, A. A.
Gallawa, J. R.
Tran, G. T.
Asebiah, D. C.
Storck, E. N.
McBride, B. C.
Miller, R. C.
Prieto, A. L.
Persson, K. A.
Toberer, E.
Stevanović, V.
Zakutayev, A.
Neilson, J. R.
2024

Recent computational studies have predicted many new ternary nitrides, revealing synthetic opportunities in this underexplored phase space. However, synthesizing new ternary nitrides is difficult, in part because intermediate and product phases often have high cohesive energies that inhibit diffusion. Here, we report the synthesis of two new phases, calcium zirconium nitride (CaZrN2) and calcium hafnium nitride (CaHfN2), by solid state metathesis reactions between Ca3N2 and ...

Jobflow: Computational Workflows Made Simple

Rosen, A. S.
Gallant, M.
George, J.
Riebesell, J.
Sahasrabuddhe, H.
Shen, J.-X.
Wen, M.
Evans, M. L.
Petretto, G.
Waroquiers, D.
Rignanese, G.-M.
Persson, K. A.
Jain, A.
Ganose, A. M.
2024

We present Jobflow, a domain-agnostic Python package for writing computational workflows tailored for high-throughput computing applications. With its simple decorator-based approach, functions and class methods can be transformed into compute jobs that can be stitched together into complex workflows. Jobflow fully supports dynamic workflows where the full acyclic graph of compute jobs is not known until runtime, such as compute jobs that launch other jobs based on the results of previous steps in the workflow. The results of all Jobflow compute jobs can be easily stored in a variety of...

A Critical Analysis of Chemical and Electrochemical Oxidation Mechanisms in Li-Ion Batteries

Spotte-Smith, E. W. C.
Vijay, S.
Petrocelli, T. B.
Rinkel, B. L. D.
McCloskey, B. D.
Persson, K. A.
2024

Electrolyte decomposition limits the lifetime of commercial lithium-ion batteries (LIBs) and slows the adoption of next-generation energy storage technologies. A fundamental understanding of electrolyte degradation is critical to rationally design stable and energy-dense LIBs. To date, most explanations for electrolyte decomposition at LIB positive electrodes have relied on ethylene carbonate (EC) being chemically oxidized by evolved singlet oxygen (1O2) or electrochemically oxidized. In this work, we apply density functional theory...