Enhanced Durability of Ca Metal Battery with Dual Salt: Synergistic Effect on Solid Electrolyte Interphase and Solvation Structure for Improved Electrodeposition.

The use of Ca metal in battery technology is a promising approach owing to its high energy density and sustainability. However, the increased battery resistance during extended cycling significantly narrows its application range. This study aimed to improve the long-term stability of Ca deposition by employing a dual-salt strategy based on calcium monocarborane, Ca(CBH), which demonstrated favorable Ca deposition characteristics as a single-salt electrolyte.

Highly Ordered Bimodal Mesoporous Carbon from ABC Triblock Terpolymers with Phenolic Resol.

Mesoporous carbons (MPCs) with a bimodal distribution of pore diameters are more advantageous than their monomodal counterparts for applications in adsorption, catalysis, and drug delivery systems; however, reports on their fabrication remain limited. In this study, we successfully fabricated bimodal MPCs using a soft template method with poly(2,2,2-trifluoroethyl methacrylate) (PTFEMA)--poly(4-vinylpyridine) (P4VP)--polystyrene (PS) and resol. The blend samples formed microphase-separated structures comprising PTFEMA spheres, PS cylinders, and matrix domains composed of P4VP and resol, leading to the separation of the PTFEMA and PS domains.

Small-angle X-ray scattering analysis of poly(amic acid) dispersed in a liquid matrix to understand the size control of polyimide nanoparticles.

Poly(amic ‍acid) ‍nanoparticles ‍prepared ‍by ‍‍precipitation ‍polymerization with a dispersant were evaluated by small-angle X-ray scattering (SAXS) and field-emission scanning electron microscopy (FE-SEM). The particle size evaluation of poly(amic acid) nanoparticles in the liquid phase by SAXS was performed to gain insight into the size control of poly(amic acid) nanoparticles, and showed good agreement with visual observation by FE-SEM, explaining the effect of the dispersant in obtaining polyimide nanoparticles with small particle size. This indicates that the particle size is maintained without change during the solvent evaporation process.

Chemically tailored block copolymers for highly reliable sub-10-nm patterns by directed self-assembly.

While block copolymer (BCP) lithography is theoretically capable of printing features smaller than 10 nm, developing practical BCPs for this purpose remains challenging. Herein, we report the creation of a chemically tailored, highly reliable, and practically applicable block copolymer and sub-10-nm line patterns by directed self-assembly. Polystyrene-block-[poly(glycidyl methacrylate)-random-poly(methyl methacrylate)] (PS-b-(PGMA-r-PMMA) or PS-b-PGM), which is based on PS-b-PMMA with an appropriate amount of introduced PGMA (10-33 mol%) is quantitatively post-functionalized with thiols.

Core-Shell Double Gyroids Directed by Selective Solvation for ABC Triblock Terpolymers.

The formation of ABC triblock terpolymers through solution casting is still challenging. In this study, core-shell double gyroid network structures are fabricated via solution casting using poly(2,2,2-trifluoroethyl methacrylate) (PTFEMA) (F)-b-[poly(4-vinylpyridine) (P4VP) (P)]-b-[polystyrene (PS) (S)] (FPS) triblock terpolymers in N,N-dimethylformamide (DMF). Upon heat treatment, the polymer tends to form a sphere-in-lamellar structure at the F/S interface.

Prediction of Photochromism of Salicylideneaniline Crystals Using a Data Mining Approach.

Salicylideneanilines (SAs) are photochromic compounds that undergo enol-keto photoisomerization in the solid state. Research over the past 60 years has revealed empirically that SAs with steric and planar conformations tend to be photochromic and nonphotochromic, respectively. However, increasing counterexamples in the recent literature raise questions about the nature of the relationship between structure and photochromism in SA crystals and whether the photochromism of SA crystals is predictable.

Redox: Organic Robust Radicals and Their Polymers for Energy Conversion/Storage Devices.

Persistent radicals can hold their unpaired electrons even under conditions where they accumulate, leading to the unique characteristics of radical ensembles with open-shell structures and their molecular properties, such as magneticity, radical trapping, catalysis, charge storage, and electrical conductivity. The molecules also display fast, reversible redox reactions, which have attracted particular attention for energy conversion and storage devices. This paper reviews the electrochemical aspects of persistent radicals and the corresponding macromolecules, radical polymers.

Extracting higher-conductivity designs for solid polymer electrolytes by quantum-inspired annealing.

Data-driven optimal structure exploration has become a hot topic in materials for energy-related devices. However, this method is still challenging due to the insufficient prediction accuracy of material properties and large exploration space for candidate structures. We propose a data trend analysis system for materials using quantum-inspired annealing.

Charge-transport kinetics of dissolved redox-active polymers for rational design of flow batteries.

Charge-transport kinetics of redox-active polymers is essential in designing electrochemical devices. We formulate the homogeneous and heterogeneous charge-transfer processes of the redox-active polymers dissolved in electrolytes. The critical electrochemical parameters, the apparent diffusion coefficient of charge transport ( ) and standard electrochemical reaction constant ( ), are estimated by considering the physical diffusion of polymer chains ( , ∝ ).

Automated Design of Li -Conducting Polymer by Quantum-Inspired Annealing.

Automated molecule design by computers is an essential topic in materials informatics. Still, generating practical structures is not easy because of the difficulty in treating material stability, synthetic difficulty, mechanical properties, and other miscellaneous parameters, often leading to the generation of junk molecules. The problem is tackled by introducing supervised/unsupervised machine learning and quantum-inspired annealing.

A PROXYL-Type Norbornene Polymer for High-Voltage Cathodes in Lithium Batteries.

A newly designed radical polymer with a polynorbornene backbone and unsaturated derivative of tetramethylpyrrolidine 1-oxyl (PROXYL) as pendant groups displays reversible redox at 3.75 V (vs Li/Li ). The robust polymer design enables the high voltage while maintaining a promising cyclability (over 1000 cycles).

Generative Models for Extrapolation Prediction in Materials Informatics.

We report a deep generative model for regression tasks in materials informatics. The model is introduced as a component of a data imputer and predicts more than 20 diverse experimental properties of organic molecules. The imputer is designed to predict material properties by "imagining" the missing data in the database, enabling the use of incomplete material data.

TEMPO-Substituted Poly(ethylene sulfide) for Solid-State Electro-Chemical Charge Storage.

A poly(ethylene sulfide) backbone is introduced as the main chain of a radical polymer. Anionic ring-opening polymerization of an episulfide monomer substituted with 2,2,6,6tetramethylpiperidin1oxyl (TEMPO), a robust nitroxide radical, yields the corresponding polythioether. Compared to the traditional poly(ethylene oxide) backbone, the new polymer shows a lower glass transition temperature (-10 °C), and about threefold higher solid-state ionic conductivity.

AI-Assisted Exploration of Superionic Glass-Type Li Conductors with Aromatic Structures.

It has long remained challenging to predict the properties of complex chemical systems, such as polymer-based materials and their composites. We have constructed the largest database of lithium-conducting solid polymer electrolytes (10 entries) and employed a transfer-learned graph neural network to accurately predict their conductivity (mean absolute error of less than 1 on a logarithmic scale). The bias-free prediction by the network helped us to find superionic conductors composed of charge-transfer complexes of aromatic polymers (ionic conductivity of around 10 S/cm at room temperature).

Metal-Free, Solid-State, Paperlike Rechargeable Batteries Consisting of Redox-Active Polyethers.

Metal-free and totally organic based batteries were fabricated from functional polyethers. Aliphatic polyethers, in which 2,2,6,6-tetramethylpiperidin-1-oxyl and viologen were introduced with high density, were used as the cathode and anode active materials, respectively. By stacking nanosheets of the polymers and an imidazolium-substituted polyether as the electrolyte, a solid-state cell only 2 μm thick was made.

Facile Synthesis of Poly(Glycidyl Ether)s with Ionic Pendant Groups by Thiol-Ene Reactions.

Poly(glycidyl ether)s having trifluoromethanesulfonylimide or imidazolium pendant groups are synthesized by thiol-ene reactions. The precise synthesis of a precursor polymer, poly(allyl glycidyl ether), and the following click reactions enable the facile preparation of the polyelectrolytes with the controlled length of main and side chains. The low glass transition temperature (<<0 °C) of the polyethers is beneficial to provide a conductivity as high as 10 S cm at room temperature, without compositing any additives.

Ultrathin and Stretchable Rechargeable Devices with Organic Polymer Nanosheets Conformable to Skin Surface.

Ultrathin flexible electronic devices have been attracting substantial attention for biomonitoring, display, wireless communication, and many other ubiquitous applications. In this article, organic robust redox-active polymer/carbon nanotube hybrid nanosheets with thickness of just 100 nm are reported as power sources for ultrathin devices conformable to skin. Regardless of the extreme thinness of the electrodes, a moderately large current density of 0.

An Ultrahigh Output Rechargeable Electrode of a Hydrophilic Radical Polymer/Nanocarbon Hybrid with an Exceptionally Large Current Density beyond 1 A cm.

Facile charge transport by a hydrophilic organic radical-substituted polymer and the 3D current collection by a self-assembled mesh of single-walled carbon nanotube bundles lead to the operation of an ultrahigh-output rechargeable electrode. Exceptionally large current density beyond 1 A cm and high areal capacity around 3 mAh cm are achieved, which are 10 times larger than those of the previously reported so-called "ultrafast electrodes." A sub-millimeter-thick, flexible, highly safe organic redox polymer-based rechargeable device with an aqueous sodium chloride electrolyte is fabricated to demonstrate the superior performance.