2021 New's Items

Prospects for Employing Lithium Copper Phosphates as High-Voltage Li-Ion Cathodes

Vincent RC, ,
Shen J-X
Preefer MB
Preefer MB
Lin J
Seeler F
Schierle-Arndt K
Persson KA
Seshadri R
2021

Three compositions of lithium copper phosphates: Li2CuPO4, Li2Cu5(PO4)4, and Li2CuP2O7 have been studied as potential high-voltage cathode materials for Li-ion batteries, following computational predictions of high operating voltages. An assisted-microwave preparation of Li2CuPO4, which is otherwise...

Promises and Challenges of Next-Generation “Beyond Li-ion” Batteries for Electric Vehicles and Grid Decarbonization

Tian Y
Zeng G
Rutt A
Shi T
Kim H
Wang J
Koettgen J
Sun Y
Ouyang B
Chen T
Lun Z
Rong Z
Persson KA
Ceder G
2021

The tremendous improvement in performance and cost of lithium-ion batteries (LIBs) have made them the technology of choice for electrical energy storage. While established battery chemistries and cell architectures for Li-ion batteries achieve good power and energy density, LIBs are unlikely to meet all the performance, cost, and scaling targets required for energy storage, in particular, in large-scale applications such as electrified transportation and grids. The demand to further reduce cost and/or increase energy density, as well as the growing concern related to natural resource...

Lowering Ternary Oxide Synthesis Temperatures by Solid-State Cometathesis Reactions

Wustrow A
Huang G
McDermott MJ
O’Nolan D
Liu C-H
Tran GT
McBride BC
Dwaraknath SS
Chapman KW
Billinge SJL
Persson KA
Thornton K
Neilson JR
2021

Low-temperature synthesis routes are necessary for selectively synthesizing many metastable solid-state materials. Here, we identify a cooperative effect that starting materials have in lowering temperatures in solid-state metathesis reactions by studying the formation of yttrium manganese oxide. Previous studies have shown that YMnO3 can be synthesized by ternary metathesis with an alkali halide being produced as a secondary product. In this contribution, we show that by using alkaline earth metals instead of alkali metals, the polymorph selectivity of the...

Ion Correlations and Their Impact on Transport in Polymer-Based Electrolytes

Fong KD
Self J
McCloskey BD
Persson KA
2021

The development of next-generation polymer-based electrolytes for energy storage applications would greatly benefit from a deeper understanding of transport phenomena in these systems. In this Perspective, we argue that the Onsager transport equations provide an intuitive but underutilized framework for analyzing transport in polymer-based electrolytes. Unlike the ubiquitous Stefan–Maxwell equations, the Onsager framework generates transport coefficients with clear physical interpretation at the atomistic level and can be computed easily from molecular simulations using Green–Kubo...

Insight into SEI Growth in Li-Ion Batteries using Molecular Dynamics and Accelerated Chemical Reactions

Alzate-Vargas L
Blau SM
Spotte-Smith EWC
Allu S
Persson KA
Fattebert J-L
2021

The performance of lithium-ion batteries (LIB) using organic electrolytes strongly depends on the formation of a stable solid electrolyte interphase (SEI) film. Elucidating the dynamic evolution and spatial composition of the SEI can be very useful to study the stability of SEI components and help optimize the formation cycles of LIB. We propose a classical molecular dynamics simulation protocol for predicting the first stages of SEI formation using a reaction method involving the decomposition of EC and LiPF6 molecules in the electrolyte. We accelerate the...

Efficient calculation of carrier scattering rates from first principles

Ganose AM
Park J
Faghaninia A
Woods-Robinson R
Persson KA
Jain A
2021

The electronic transport behaviour of materials determines their suitability for technological applications. We develop a computationally efficient method for calculating carrier scattering rates of solid-state semiconductors and insulators from first principles inputs. The present method extends existing polar and non-polar electron-phonon coupling, ionized impurity, and piezoelectric scattering mechanisms formulated for isotropic band structures to support highly anisotropic materials. We test the formalism by calculating the electronic transport properties of 23 semiconductors,...

Effective Local Geometry Descriptor for 29Si NMR Q4 Anisotropy

Venetos MC
Dwaraknath S
Persson KA
2021

The nuclear shielding anisotropy, ζ, is a useful nuclear magnetic resonance (NMR) shielding tensor parameter in describing the extent of electron cloud distortion about an atom. Despite the advantages afforded by NMR in structural characterization, the relationship between ζ and local structure of an atom in high-symmetry environments, such as Si–Q4 sites, is poorly understood. Here, we use a data-driven approach combining random forest feature ranking and the Sure Independence Screening and Sparsifying Operator (SISSO) approach to derive a simple and...

Database of ab initio L-edge X-ray absorption near edge structure

Chen Y
Chen C
Zheng C
Dwaraknath S
Horton MK
Cabana J
Rehr J
Vinson J
Dozier A
Kas JJ
Persson KA
Ong SP
2021

The L-edge X-ray Absorption Near Edge Structure (XANES) is widely used in the characterization of transition metal compounds. Here, we report the development of a database of computed L-edge XANES using the multiple scattering theory-based FEFF9 code. The initial release of the database contains more than 140,000 L-edge spectra for more than 22,000 structures generated using a high-throughput computational workflow. The data is disseminated through the Materials Project and addresses a critical need for L-edge XANES spectra among the research community.

Data-Driven Prediction of Formation Mechanisms of Lithium Ethylene Monocarbonate with an Automated Reaction Network

Xie X
Clark Spotte-Smith EW
Wen M
Patel HD
Blau SM
Persson KA
2021

Interfacial reactions are notoriously difficult to characterize, and robust prediction of the chemical evolution and associated functionality of the resulting surface film is one of the grand challenges of materials chemistry. The solid–electrolyte interphase (SEI), critical to Li-ion batteries (LIBs), exemplifies such a surface film, and despite decades of work, considerable controversy remains regarding the major components of the SEI as well as their formation mechanisms. Here we use a reaction network to investigate whether lithium ethylene monocarbonate (LEMC) or lithium...

BonDNet: a graph neural network for the prediction of bond dissociation energies for charged molecules

Wen M
Blau SM
Spotte-Smith EWC
Dwaraknath S
Persson KA
2021

A broad collection of technologies, including e.g. drug metabolism, biofuel combustion, photochemical decontamination of water, and interfacial passivation in energy production/storage systems rely on chemical processes that involve bond-breaking molecular reactions. In this context, a fundamental thermodynamic property of interest is the bond dissociation energy (BDE) which measures the strength of a chemical bond. Fast and accurate prediction of BDEs for arbitrary molecules would lay the groundwork for data-driven projections of complex reaction cascades and hence a deeper...