Discovery of novel Li SSE and anode coatings using interpretable machine learning and high-throughput multi-property screening.

All-solid-state batteries with Li metal anode can address the safety issues surrounding traditional Li-ion batteries as well as the demand for higher energy densities. However, the development of solid electrolytes and protective anode coatings possessing high ionic conductivity and good stability with Li metal has proven to be a challenge. Here, we present our informatics approach to explore the Li compound space for promising electrolytes and anode coatings using high-throughput multi-property screening and interpretable machine learning. To do this, we generate a database of battery-related materials properties by computing [Formula: see text] migration barriers and stability windows for over 15,000 Li-containing compounds from Materials Project. We screen through the database for candidates with good thermodynamic and electrochemical stabilities, and low [Formula: see text] migration barriers, identifying promising new candidates such as [Formula: see text]N, [Formula: see text], [Formula: see text], [Formula: see text], and [Formula: see text], among others. We train machine learning models, using ensemble methods, to predict migration barriers and oxidation and reduction potentials of these compounds by engineering input features that ensure accuracy and interpretability. Using only a small number of features, our gradient boosting regression models achieve [Formula: see text] values of 0.95 and 0.92 on the oxidation and reduction potential prediction tasks, respectively, and 0.86 on the migration barrier prediction task. Finally, we use Shapley additive explanations and permutation feature importance analyses to interpret our machine learning predictions and identify materials properties with the largest impact on predictions in our models. We show that our approach has the potential to enable rapid discovery and design of novel solid electrolytes and anode coatings.

Thermal runaway of Lithium-ion batteries employing LiN(SO2F)2-based concentrated electrolytes.

Concentrated electrolytes usually demonstrate good electrochemical performance and thermal stability, and are also supposed to be promising when it comes to improving the safety of lithium-ion batteries due to their low flammability. Here, we show that LiN(SO2F)2-based concentrated electrolytes are incapable of solving the safety issues of lithium-ion batteries. To illustrate, a mechanism based on battery material and characterizations reveals that the tremendous heat in lithium-ion batteries is released due to the reaction between the lithiated graphite and LiN(SO2F)2 triggered thermal runaway of batteries, even if the concentrated electrolyte is non-flammable or low-flammable. Generally, the flammability of an electrolyte represents its behaviors when oxidized by oxygen, while it is the electrolyte reduction that triggers the chain of exothermic reactions in a battery. Thus, this study lights the way to a deeper understanding of the thermal runaway mechanism in batteries as well as the design philosophy of electrolytes for safer lithium-ion batteries.

Microstructural observation of fuel cell catalyst inks by Cryo-SEM and Cryo-TEM.

In order to improve the electricity generation performance of fuel cell electric vehicles, it is necessary to optimize the microstructure of the catalyst layer of a polymer electrolyte fuel cell. The catalyst layer is formed by a wet coating process using catalyst inks. Therefore, it is very important to observe the microstructure of the catalyst ink. In this study, the morphology of carbon-supported platinum (Pt/C) particles in catalyst inks with a different solvent composition was investigated by cryogenic scanning electron microscopy (cryo-SEM). In addition, the morphology of the ionomer, which presumably influences the formation of agglomerated Pt/C particles in a catalyst ink, was investigated by cryogenic transmission electron microscopy (cryo-TEM). The results of a cryo-SEM observation revealed that the agglomerated Pt/C particles tended to become coarser with a higher 1-propanol (NPA) weight fraction. The results of a cryo-TEM observation indicated that the actual ionomer dispersion in a catalyst ink formed a network structure different from that of the ionomer in the solvent.

Measurement of a new parameter representing the gas transport properties of the catalyst layers of polymer electrolyte fuel cells.

The optimization of the catalyst layers is necessary for obtaining a better fuel cell performance and reducing fuel cell cost. Although the ionomer coverage of the Pt catalyst is said to be a key parameter in this regard, the proportion of Pt either directly or indirectly covered by the ionomer is thought to be an important parameter with regard to gas transport (indirectly covered Pt: its gas transport paths are completely blocked by the ionomer even if it does not directly cover Pt). In this study, a new technique has been developed for evaluating the proportion of Pt covered indirectly or directly by the ionomer, which is defined as the "capped proportion", based on the carbon monoxide (CO) adsorption properties at different temperatures. The validity of the method was thoroughly examined by identifying the CO adsorption properties of the components of the catalyst layers. The capped proportion and oxygen transport resistance in the catalyst layers showed a good correlation, indicating that the capped proportion is a dominant factor of oxygen transport resistance. This technique thus enables the evaluation of the dominant factor of the gas transport properties of the catalyst layers. The method has another significant advantage in that it does not require a membrane electrode assembly, let alone electrochemical measurement, which should be helpful for catalyst layer optimization.

Surface oxide growth on platinum electrode in aqueous trifluoromethanesulfonic acid.

Platinum in the form of nanoparticles is the key and most expensive component of polymer electrolyte membrane fuel cells, while trifluoromethanesulfonic acid (CF3SO3H) is the smallest fluorinated sulfonic acid. Nafion, which acts as both electrolyte and separator in fuel cells, contains -CF2SO3H groups. Consequently, research on the electrochemical behaviour of Pt in aqueous CF3SO3H solutions creates important background knowledge that can benefit fuel cell development. In this contribution, Pt electro-oxidation is studied in 0.1 M aqueous CF3SO3H as a function of the polarization potential (E(p), 1.10 ≤ E(p) ≤ 1.50 V), polarization time (t(p), 10(0) ≤ t(p) ≤ 10(4) s), and temperature (T, 278 ≤ T ≤ 333 K). The critical thicknesses (X1), which determines the applicability of oxide growth theories, is determined and related to the oxide thickness (d(ox)). Because X1 > d(ox) for the entire range of E(p), t(p), and T values, the formation of Pt surface oxide follows the interfacial place-exchange or the metal cation escape mechanism. The mechanism of Pt electro-oxidation is revised and expanded by taking into account possible interactions of cations, anions, and water molecules with Pt. A modified kinetic equation for the interfacial place exchange is proposed. The application of the interfacial place-exchange and metal cation escape mechanisms leads to an estimation of the Pt(δ+)-O(δ-) surface dipole (µ(PtO)), and the potential drop (V(ox)) and electric field (E(ox)) within the oxide. The Pt-anion interactions affect the oxidation kinetics by indirectly influencing the electric field within the double layer and the surface oxide.