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Lithium bis(fluorosulfonyl)imide-based liquid electrolytes are promising for realizing high coulombic efficiency and long cycle life in next-generation Li-metal batteries. However, the role of anions in the formation of the solid-electrolyte interphase remains unclear. Here we combine electrochemical analyses and X-ray photoelectron spectroscopy measurements, both with and without sample washing, together with computational simulations, to propose the reaction pathways of electrolyte decomposition and correlate the interphase component solubility with the efficacy of passivation. We discover that not all the products derived from interphase-forming reactions are incorporated into the resulting passivation layer, with a notable portion present in the liquid electrolyte. We also find that the high-performance electrolytes can afford a sufficiently passivating interphase with minimized electrolyte decomposition, by incorporating more anion-decomposition products. Overall, this work presents a systematic approach of coupling electrochemical and surface analyses to paint a comprehensive picture of solid-electrolyte interphase formation, while identifying the key attributes of high-performance electrolytes to guide future designs.

Humans rely increasingly on sensors to address grand challenges and to improve quality of life in the era of digitalization and big data. For ubiquitous sensing, flexible sensors are developed to overcome the limitations of conventional rigid counterparts. Despite rapid advancement in bench-side research over the last decade, the market adoption of flexible sensors remains limited. To ease and to expedite their deployment, here, we identify bottlenecks hindering the maturation of flexible sensors and propose promising solutions. We first analyze challenges in achieving satisfactory sensing performance for real-world applications and then summarize issues in compatible sensor-biology interfaces, followed by brief discussions on powering and connecting sensor networks. Issues en route to commercialization and for sustainable growth of the sector are also analyzed, highlighting environmental concerns and emphasizing nontechnical issues such as business, regulatory, and ethical considerations. Additionally, we look at future intelligent flexible sensors. In proposing a comprehensive roadmap, we hope to steer research efforts towards common goals and to guide coordinated development strategies from disparate communities. Through such collaborative efforts, scientific breakthroughs can be made sooner and capitalized for the betterment of humanity.

Neurotransmitters play essential roles in regulating neural circuit dynamics both in the central nervous system as well as at the peripheral, including the gastrointestinal tract1-3. Their real-time monitoring will offer critical information for understanding neural function and diagnosing disease1-3. However, bioelectronic tools to monitor the dynamics of neurotransmitters in vivo, especially in the enteric nervous systems, are underdeveloped. This is mainly owing to the limited availability of biosensing tools that are capable of examining soft, complex and actively moving organs. Here we introduce a tissue-mimicking, stretchable, neurochemical biological interface termed NeuroString, which is prepared by laser patterning of a metal-complexed polyimide into an interconnected graphene/nanoparticle network embedded in an elastomer. NeuroString sensors allow chronic in vivo real-time, multichannel and multiplexed monoamine sensing in the brain of behaving mouse, as well as measuring serotonin dynamics in the gut without undesired stimulations and perturbing peristaltic movements. The described elastic and conformable biosensing interface has broad potential for studying the impact of neurotransmitters on gut microbes, brain-gut communication and may ultimately be extended to biomolecular sensing in other soft organs across the body.

Designing a stable solid-electrolyte interphase on a Li anode is imperative to developing reliable Li metal batteries. Herein, we report a suspension electrolyte design that modifies the Li+ solvation environment in liquid electrolytes and creates inorganic-rich solid-electrolyte interphases on Li. Li2O nanoparticles suspended in liquid electrolytes were investigated as a proof of concept. Through theoretical and empirical analyses of Li2O suspension electrolytes, the roles played by Li2O in the liquid electrolyte and solid-electrolyte interphases of the Li anode are elucidated. Also, the suspension electrolyte design is applied in conventional and state-of-the-art high-performance electrolytes to demonstrate its applicability. Based on electrochemical analyses, improved Coulombic efficiency (up to ~99.7%), reduced Li nucleation overpotential, stabilized Li interphases and prolonged cycle life of anode-free cells (~70 cycles at 80% of initial capacity) were achieved with the suspension electrolytes. We expect this design principle and our findings to be expanded into developing electrolytes and solid-electrolyte interphases for Li metal batteries.

Shape memory polymers are promising materials in many emerging applications due to their large extensibility and excellent shape recovery. However, practical application of these polymers is limited by their poor energy densities (up to ∼1 MJ/m3). Here, we report an approach to achieve a high energy density, one-way shape memory polymer based on the formation of strain-induced supramolecular nanostructures. As polymer chains align during strain, strong directional dynamic bonds form, creating stable supramolecular nanostructures and trapping stretched chains in a highly elongated state. Upon heating, the dynamic bonds break, and stretched chains contract to their initial disordered state. This mechanism stores large amounts of entropic energy (as high as 19.6 MJ/m3 or 17.9 J/g), almost six times higher than the best previously reported shape memory polymers while maintaining near 100% shape recovery and fixity. The reported phenomenon of strain-induced supramolecular structures offers a new approach toward achieving high energy density shape memory polymers.

Next-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance. This is enabled by covalently-embedded in-situ rubber matrix (iRUM) formation through good mixing of iRUM precursors with polymer electronic materials, and finely-controlled composite film morphology built on azide crosslinking chemistry which leverages different reactivities with C-H and C=C bonds. The high covalent crosslinking density results in both superior elasticity and solvent resistance. When applied in stretchable transistors, the iRUM-semiconductor film retained its mobility after stretching to 100% strain, and exhibited record-high mobility retention of 1 cm2 V-1 s-1 after 1000 stretching-releasing cycles at 50% strain. The cycling life was stably extended to 5000 cycles, five times longer than all reported semiconductors. Furthermore, we fabricated elastic transistors via consecutively photo-patterning of the dielectric and semiconducting layers, demonstrating the potential of solution-processed multilayer device manufacturing. The iRUM represents a molecule-level design approach towards robust skin-inspired electronics.

Translating all-polymer solar cells from spin-coating to scalable roll-to-roll-compatible fabrication techniques is a critical step toward the application of organic photovoltaics at a scale. Techniques to control polymer crystallization and phase separation during solution printing are essential to obtain high-performance printed organic solar cells. Here, we demonstrate a novel solvent additive approach employing trace amounts of phthalates as additives to control polymer crystallinity and suppress unfavorable phase separation in a representative PTB7-Th/P(NDI2OD-2T) all-polymer solar cell. The best-performing additive increased the blade-coated device performance from 2.09 to 4.50% power conversion efficiency, an over twofold improvement, mitigating the loss in performance that is typically observed during process transfer from spin-coating to blade-coating. It is suggested that the improved device performance stems from a finer polymer phase-separation size and overall improved active layer morphology, evidenced by device characterization data and indirectly supported by grazing incidence wide-angle X-ray scattering analyses. Real-time X-ray diffraction measurements during blade-coating provide mechanistic insights and suggest that the dioctyl phthalate additive may act as a compatibilizer, reducing the demixing of the donor and acceptor polymer during film formation, enabling a smaller phase separation and improved performance. The structural diversity of the class of phthalate additives makes this simple yet effective concept promising for translating other all-polymer material systems to blade-coating and other scalable printing techniques.

Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal-organic framework consisting of M-N4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB's catalytic activity, and they suggest that M-HAB's organic linker acts as the active site with the role of the metal being to modulate the linker sites' binding strength.

Abstract: A major hurdle to the successful deployment of high‐energy‐density lithium metal based batteries is dendrite growth during battery cycling, which raises safety and cycle life concerns. Coating the Li metal anode with a soft polymer layer has been previously shown to be effective in suppressing dendrite growth, leading to uniform lithium deposition even at high current densities. A 3D coarse‐grained molecular model to study the mechanism of dendrite suppression is presented. It is found that the most effective coatings delay or even prevent dendrites from penetrating the polymer layer during deposition. The optimal deposition can be achieved by jointly tuning the polymer stiffness and relaxation time. Higher polymer dielectric permittivity and coating thickness are also effective, but the deposition rate and, therefore, the charging current density is reduced. These findings provide the basis for rational design of soft polymer coatings for stable lithium deposition.

The structural and functional complexity of multicellular biological systems, such as the brain, are beyond the reach of human design or assembly capabilities. Cells in living organisms may be recruited to construct synthetic materials or structures if treated as anatomically defined compartments for specific chemistry, harnessing biology for the assembly of complex functional structures. By integrating engineered-enzyme targeting and polymer chemistry, we genetically instructed specific living neurons to guide chemical synthesis of electrically functional (conductive or insulating) polymers at the plasma membrane. Electrophysiological and behavioral analyses confirmed that rationally designed, genetically targeted assembly of functional polymers not only preserved neuronal viability but also achieved remodeling of membrane properties and modulated cell type-specific behaviors in freely moving animals. This approach may enable the creation of diverse, complex, and functional structures and materials within living systems.

The next materials challenge in organic stretchable electronics is the development of a fully degradable semiconductor that maintains stable electrical performance under strain. Herein, we decouple the design of stretchability and transience by harmonizing polymer physics principles and molecular design in order to demonstrate for the first time a material that simultaneously possesses three disparate attributes: semiconductivity, intrinsic stretchability, and full degradability. We show that we can design acid-labile semiconducting polymers to appropriately phase segregate within a biodegradable elastomer, yielding semiconducting nanofibers that concurrently enable controlled transience and strain-independent transistor mobilities. Along with the future development of suitable conductors and device integration advances, we anticipate that these materials could be used to build fully biodegradable diagnostic or therapeutic devices that reside inside the body temporarily, or environmental monitors that are placed in the field and break down when they are no longer needed. This fully degradable semiconductor represents a promising advance toward developing multifunctional materials for skin-inspired electronic devices that can address previously inaccessible challenges and in turn create new technologies.

State-of-the-art lithium (Li)-ion batteries are approaching their specific energy limits yet are challenged by the ever-increasing demand of today’s energy storage and power applications, especially for electric vehicles. Li metal is considered an ultimate anode material for future high-energy rechargeable batteries when combined with existing or emerging high-capacity cathode materials. However, much current research focuses on the battery materials level, and there have been very few accounts of cell design principles. Here we discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg −1 , up to 500 Wh kg −1 , for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials. We also provide an analysis of key factors such as cathode loading, electrolyte amount and Li foil thickness that impact the cell-level cycle life. Furthermore, we identify several important strategies to reduce electrolyte-Li reaction, protect Li surfaces and stabilize anode architectures for long-cycling high-specific-energy cells.

Dielectric elastomer actuators (DEAs) offer versatile applications including haptics, soft robotics and smart lenses. However, due to the lack of conductive electrodes with low modulus and high stretchability, their use is limited by nonsolid electrodes, hindering integration with other systems. In this study, transparent and patternable solid electrodes, achieving actuation performance comparable to a commonly used non‐solid counterpart (e.g., carbon grease), with a stretchable and patternable conducting polymer composed of PEDOT:PSS and PEG‐PPG‐PEG diacrylate (P123DA) are reported. Varying the ratio of P123DA to PEDOT:PSS enables optimization of electrical and mechanical properties to achieve compliant solid electrodes in static and dynamic actuation. The ratio of P123DA to PEDOT:PSS is found to impact PEDOT:PSS nanofiber formation and the associated electrical and mechanical properties. Moreover, the resulting P123DA/PEDOT:PSS‐based solid electrode shows excellent optical transmittance exceeding 95%. This work highlights the potential of tuning different solid electrode properties to realize transparent, patternable, and stretchable solid electrodes, enhancing their applicability in diverse fields. [ABSTRACT FROM AUTHOR]