2024 New's Items

Chemical Origin of in Situ Carbon Dioxide Outgassing from a Cation-Disordered Rock Salt Cathode

Huang T-Y
Cai Z
Crafton MJ
Giovine R
Patterson A
Hau H-M
2024

In situ carbon dioxide (CO2) outgassing is a common phenomenon in lithium-ion batteries (LiBs), primarily due to parasitic side reactions at the cathode–electrolyte interface. However, little is known about the chemical origins of the in situ CO2 released from emerging Li-excess cation-disordered rock salt (DRX) cathodes. In this study, we selectively labeled various carbon sources with 13C in cathodes containing a representative DRX material, Li1.2Mn0.4Ti...

AlabOS: a Python-based reconfigurable workflow management framework for autonomous laboratories

Fei Y
Rendy B
Kumar R
Dartsi O
Sahasrabuddhe HP
McDermott MJ
2025

The recent advent of autonomous laboratories, coupled with algorithms for high-throughput screening and active learning, promises to accelerate materials discovery and innovation. As these autonomous systems grow in complexity, the demand for robust and efficient workflow management software becomes increasingly critical. In this paper, we introduce AlabOS, a general-purpose software framework for orchestrating experiments and managing resources, with an emphasis on automated laboratories for materials synthesis and characterization. AlabOS features a reconfigurable experiment workflow...

Nitride Lithium-ion Conductors with Enhanced Oxidative Stability

Jun K
Xiao Y
Sun W
Byeon Y-W
Kim H
Ceder G
2024

It is desirable to develop solid electrolytes that have both excellent reductive stability against lithium metal and oxidative stability against high-voltage cathodes. However, no inorganic superionic conductors reported thus far satisfy these criteria. Nitrides exhibit intrinsically superior stability against reduction but are often readily oxidized at voltages as low as 0.6 V. In this article, we investigated all nitride-based compounds to search for materials with improved oxidative stabilities over 2.0 V while retaining their intrinsic stability against Li metal. We found two...

Earth-abundant Li-ion cathode materials with nanoengineered microstructures

Hau H-M
Mishra T
Ophus C
Huang T-Y
Bustilo K
Sun Y
2024

Manganese-based materials have tremendous potential to become the next-generation lithium-ion cathode as they are Earth abundant, low cost and stable. Here we show how the mobility of manganese cations can be used to obtain a unique nanosized microstructure in large-particle-sized cathode materials with enhanced electrochemical properties. By combining atomic-resolution scanning transmission electron microscopy, four-dimensional scanning electron nanodiffraction and in situ X-ray diffraction, we show that when a partially delithiated, high-manganese-content, disordered rocksalt cathode is...

Uncertainty-aware particle segmentation for electron microscopy at varied length scales

Rettenberger L
Szymanski NJ
Zeng Y
Schuetzke J
Wang S
Ceder G
2024

Electron microscopy is indispensable for examining the morphology and composition of solid materials at the sub-micron scale. To study the powder samples that are widely used in materials development, scanning electron microscopes (SEMs) are increasingly used at the laboratory scale to generate large datasets with hundreds of images. Parsing these images to identify distinct particles and determine their morphology requires careful analysis, and automating this process remains challenging. In this work, we enhance the Mask R-CNN architecture to develop a method for automated...

Effect of Cation Disorder on Lithium Transport in Halide Superionic Conductors

Zhong P
Gupta S
Deng B
Jun K
Ceder G
2024

Li2ZrCl6 (LZC) is a promising solid-state electrolyte due to its affordability, moisture stability, and high ionic conductivity. We computationally investigate the role of cation disorder in LZC and its effect on Li-ion transport by integrating thermodynamic and kinetic modeling. The results demonstrate that fast Li-ion conductivity requires Li-vacancy disorder, which is dependent on the degree of Zr disorder. The high temperature required to form equilibrium Zr disorder precludes any equilibrium synthesis processes for achieving fast Li-ion conductivity,...

Revealing Dynamic Evolution of the Anode-Electrolyte Interphase in All-Solid-State Batteries with Excellent Cyclability

Kim SY
Bak S
Jun K
Ceder G
Chen G
2024

All-solid-state-batteries (ASSBs) based on a halide solid electrolyte (SE) and a lithium-metal based anode typically have poor cyclability without a buffer layer (such as Li3PS4 or Li6PS5Cl) to prevent the degradation reactions. Here excellent cycling stability of ASSB consisting of an uncoated single-crystal LiNi0.8Co0.1Mn0.1O2 cathode and a Li3YCl...

The Limited Incorporation and Role of Fluorine in Mn-rich Disordered Rocksalt Cathodes

Wu VC
Zhong P
Ong J
Yoshida E
Kwon A
Ceder G
2024

Disordered rocksalt oxide (DRX) cathodes are promising candidates for next-generation Co- and Ni-free Li-ion batteries. While fluorine substitution for oxygen has been explored as an avenue to enhance their performance, the amount of fluorine incorporated into the DRX structure is particularly challenging to quantify and impedes our ability to relate fluorination to electrochemical performance. Herein, an experimental–computational method combining 7Li and 19F solid-state nuclear magnetic resonance, and ab initio cluster expansion Monte Carlo simulations, is...

Fast Room-Temperature Mg-Ion Conduction in Clay-Like Halide Glassy Electrolytes

Yang X
Gupta S
Chen Y
Sari D
Hau H
Cai Z
2024

The discovery of mechanically soft solid-state materials with fast Mg-ion conduction is crucial for the development of solid-state magnesium batteries. In this paper, novel magnesium gallium halide compounds are reported that achieve high ionic conductivity of 0.47 mS cm−1 at room temperature. These Mg-ion conductors obtained by ball milling Mg and Ga salts exhibit clay-like mechanical properties, enabling intimate contact at the electrode–electrolyte interface during battery cycling. With a combination of experimental and computational analysis, this study identifies that the...

Alkali-Ion-Assisted Activation of ε-VOPO4 as a Cathode Material for Mg-Ion Batteries

Sari D
Rutt A
Kim J
Chen Q
Hahn NT
Kim H
2024

Rechargeable multivalent-ion batteries are attractive alternatives to Li-ion batteries to mitigate their issues with metal resources and metal anodes. However, many challenges remain before they can be practically used due to the low solid-state mobility of multivalent ions. In this study, a promising material identified by high-throughput computational screening is investigated, ε-VOPO4, as a Mg cathode. The experimental and computational evaluation of ε-VOPO4 suggests that it may provide an energy density of >200 Wh kg−1 based on the average...