Na-based batteries are proposed as promising energy storage candidates for beyond Li-ion technology due to the higher natural earth of Na metal. For its high capacity and low potential, Na metal may carve itself a niche when directly used as anodes. Similar to or even more problematic than Li, however, uneven plating/stripping of Na leads to dendrite formation. As the plating substrates, current collectors have a paramount influence on the Na plating/stripping behaviors. Here we propose porous Al current collectors as the plating substrate to suppress Na dendrites. Al does not alloy with Na. It is advantageous over Cu current collectors in terms of cost and weight. The interconnected porous structure can increase available surface for Na to nucleate and decrease the Na flux distribution, leading to homogeneous plating. The Na metal anodes can run for over 1000 cycles on porous Al with a low and stable voltage hysteresis and their average plating/stripping Coulombic efficiency was above 99.9%, which is greatly improved compared to planar Al. We used the porous Al for Na-O, Na-NaV(PO) cells with low Na amount and anode free Na-TiS batteries and anticipate that using this strategy can be combined with further electrolyte and cathodes to develop high performance Na-based batteries.
Solid state electrolytes are the key components for high energy density lithium ion batteries and especially for lithium metal batteries where lithium dendrite growth is an inevitable obstacle in liquid electrolytes. Solid polymer electrolytes based on a complex of polymers and lithium salts are intrinsically advantageous over inorganic electrolytes in terms of processability and film‐forming properties. But other properties such as ionic conductivity, thermal stability, mechanical modulus, and electrochemical stability need to be improved. Herein, for the first time, 2D additives using few‐layer vermiculite clay sheets as an example to comprehensively upgrade poly(ethylene oxide)‐based solid polymer electrolyte are introduced. With clay sheet additives, the polymer electrolyte exhibits improved thermal stability, mechanical modulus, ionic conductivity, and electrochemical stability along with reduced flammability and interface resistance. The composite polymer electrolyte can suppress the formation and growth of lithium dendrites in lithium metal batteries. It is anticipated that the clay sheets upgraded solid polymer electrolyte can be integrated to construct high performance solid state lithium ion and lithium metal batteries with higher energy and safety.
Solid state lithium metal batteries are the most promising next-generation power sources owing to their high energy density and safety. Solid polymer electrolytes (SPE) have gained wide attention due to the excellent flexibility, manufacturability, lightweight, and low-cost processing. However, fatal drawbacks of the SPE such as the insufficient ionic conductivity and Li + transference number at room temperature restrict their practical application. Here vertically aligned 2D sheets are demonstrated as an advanced filler for SPE with enhanced ionic conductivity, Li + transference number, mechanical modulus, and electrochemical stability, using vermiculite nanosheets as an example. The vertically aligned vermiculite sheets (VAVS), prepared by the temperature gradient freezing, provide aligned, continuous, run-through polymer-filler interfaces after infiltrating with polyethylene oxide (PEO)-based SPE. As a result, ionic conductivity as high as 1.89 × 10 −4 S cm −1 at 25 °C is achieved with Li + transference number close to 0.5. Along with their enhanced mechanical strength, Li|Li symmetric cells using VAVS-CSPE are stable over 1300 h with a low overpotential. LiFePO 4 in all-solid-state lithium metal batteries with VAVS-CSPE could deliver a specific capacity of 167 mAh g −1 at 0.1 C at 35 °C and 82% capacity retention after 200 cycles at 0.5 C.
Organic molecules and polymers have a broad range of applications in biomedical, chemical, and materials science fields. Traditional design approaches for organic molecules and polymers are mainly experimentally-driven, guided by experience, intuition, and conceptual insights. Though they have been successfully applied to discover many important materials, these methods are facing significant challenges due to the tremendous demand of new materials and vast design space of organic molecules and polymers. Accelerated and inverse materials design is an ideal solution to these challenges. With advancements in high-throughput computation, artificial intelligence (especially machining learning, ML), and the growth of materials databases, ML-assisted materials design is emerging as a promising tool to flourish breakthroughs in many areas of materials science and engineering. To date, using ML-assisted approaches, the quantitative structure property/activity relation for material property prediction can be established more accurately and efficiently. In addition, materials design can be revolutionized and accelerated much faster than ever, through ML-enabled molecular generation and inverse molecular design. In this perspective, we review the recent progresses in ML-guided design of organic molecules and polymers, highlight several successful examples, and examine future opportunities in biomedical, chemical, and materials science fields. We further discuss the relevant challenges to solve in order to fully realize the potential of ML-assisted materials design for organic molecules and polymers. In particular, this study summarizes publicly available materials databases, feature representations for organic molecules, open-source tools for feature generation, methods for molecular generation, and ML models for prediction of material properties, which serve as a tutorial for researchers who have little experience with ML before and want to apply ML for various applications. Last but not least, it draws insights into the current limitations of ML-guided design of organic molecules and polymers. We anticipate that ML-assisted materials design for organic molecules and polymers will be the driving force in the near future, to meet the tremendous demand of new materials with tailored properties in different fields.
Bendable energy-storage systems with high energy density are demanded for conformal electronics. Lithium-metal batteries including lithium-sulfur and lithium-oxygen cells have much higher theoretical energy density than lithium-ion batteries. Reckoned as the ideal anode, however, Li has many challenges when directly used, especially its tendency to form dendrite. Under bending conditions, the Li-dendrite growth can be further aggravated due to bending-induced local plastic deformation and Li-filaments pulverization. Here, the Li-metal anodes are made bending tolerant by integrating Li into bendable scaffolds such as reduced graphene oxide (r-GO) films. In the composites, the bending stress is largely dissipated by the scaffolds. The scaffolds have increased available surface for homogeneous Li plating and minimize volume fluctuation of Li electrodes during cycling. Significantly improved cycling performance under bending conditions is achieved. With the bending-tolerant r-GO/Li-metal anode, bendable lithium-sulfur and lithium-oxygen batteries with long cycling stability are realized. A bendable integrated solar cell-battery system charged by light with stable output and a series connected bendable battery pack with higher voltage is also demonstrated. It is anticipated that this bending-tolerant anode can be combined with further electrolytes and cathodes to develop new bendable energy systems.
A central challenge in expanding the genetic code of cells to incorporate non-canonical amino acids into proteins is the scalable discovery of aminoacyl-tRNA synthetase (aaRS)-tRNA pairs that are orthogonal in their aminoacylation specificity. Here we computationally identify candidate orthogonal tRNAs from millions of sequences and develop a rapid, scalable approach -named tRNA Extension (tREX) -to determine the in vivo aminoacylation status of tRNAs. Using tREX, we test 243 candidate tRNAs in Escherichia coli and identify 71 orthogonal tRNAs, covering 16 isoacceptor classes, and 23 functional orthogonal tRNA-cognate aaRS pairs. We discover five orthogonal pairs, including three highly active amber suppressors, and evolve new amino acid substrate specificities for two pairs. Finally, we use tREX to characterize a matrix of 64 orthogonal synthetase-orthogonal tRNA specificities. This work expands the number of orthogonal pairs available for genetic code expansion and provides a pipeline for the discovery of additional orthogonal pairs and a foundation for encoding the cellular synthesis of non-canonical biopolymers.Genetic code expansion enables the cellular synthesis of modified proteins via the cotranslational incorporation of non-canonical amino acids 1, 2 . Orthogonal aaRS-tRNA pairs are crucial to genetic code expansion. These pairs consist of (1) a synthetase that efficiently aminoacylates its cognate tRNA, but minimally aminoacylates endogenous tRNAs in the host organism, and (2) a tRNA that is a substrate for its cognate synthetase but is a poor substrate for endogenous synthetases 3,4 . Derivatives of orthogonal pairs that recognize blank codons (most commonly, the amber stop codon) and selectively use non-canonical amino acids (ncAAs) have been used to site-specifically incorporate numerous ncAAs into proteins 3,4 . Despite many years of effort, a limited number of orthogonal aaRS-tRNA pairs *
unfolding, [2] and skin wrinkles communicate a change in the state of the body. [3] These exquisite self-wrinkling processes typically originate from heterogeneous growth rates during the growth process, which results in compressive strains on the constrained tissues or organs and leads to mechanical instability. [5,6] Hydrogels possess water-rich structures similar to the abovementioned biological tissues and are regarded as promising scaffolds in biomedical fields. [7][8][9] Given the importance of wrinkled structures, the similarity between hydrogels and biotissue, and the important role of the programmable structure of hydrogels in potential biomedical applications, [10,11] imitating the delicate architecture of biological tissues in a biocompatible, mechanically stable wrinkled hydrogel with programmable patterns can facilitate an understanding of the effects of surface topography on biological properties and will be of benefit to humanity. In fact, motivated by the distinct functionalities of wrinkled structures in biology, material scientists have attempted to mimic this structure in artificial systems. [12][13][14][15][16][17][18][19] Consequently, a series of strategies, including swelling mismatch, [20] prepatterning treatment, [21] or coating of a second layer on the substrate, [5] have been successfully conducted to generate a compressive strain that triggers a controllable wrinkling Wrinkled hydrogels from biomass sources are potential structural biomaterials. However, for biorelated applications, engineering scalable, structure-customized, robust, and biocompatible wrinkled hydrogels with highly oriented nanostructures and controllable intervals is still a challenge. A scalable biomass material, namely cellulose, is reported for customizing anisotropic, all-cellulose, wrinkle-patterned hydrogels (AWHs) through an ultrafast, auxiliary force, acid-induced gradient dual-crosslinking strategy. Direct immersion of a prestretched cellulose alkaline gel in acid and relaxation within seconds allow quick buildup of a consecutive through-thickness modulus gradient with acid-penetration-directed dual-crosslinking, confirmed by visual 3D Raman microscopy imaging, which drives the formation of selfwrinkling structures. Moreover, guided by quantitative mechanics simulations, the structure of AWHs is found to exhibit programmable intervals and aligned nanostructures that differ between ridge and valley regions and can be controlled by tuning the prestretching strain and acid treatment time, and these AWHs successfully induce cell alignment. Thus, a new avenue is opened to fabricate polysaccharide-derived, programmable, anisotropic, wrinkled hydrogels for use as biomedical materials via a bottom-up method.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.
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