ACS Materials Au最新文献

The delivery of molecules, such as DNA, RNA, peptides, and certain hydrophilic drugs, across the epidermal barrier poses a significant obstacle. Microneedle technology has emerged as a prominent area of focus in biomedical research because of its ability to deliver a wide range of biomolecules, vaccines, medicines, and other substances through the skin. Microneedles (MNs) form microchannels by disrupting the skin's structure, which compromises its barrier function, and facilitating the easy penetration of drugs into the skin. These devices enhance the administration of many therapeutic substances to the skin, enhancing their stability. Transcutaneous delivery of medications using a microneedle patch offers advantages over conventional drug administration methods. Microneedles containing active substances can be stimulated by different internal and external factors to result in the regulated release of the substances. To achieve efficient drug administration to the desired location, it is necessary to consider the design of needles with appropriate optimized characteristics. The choice of materials for developing and manufacturing these devices is vital in determining the pharmacodynamics and pharmacokinetics of drug delivery. This article provides the most recent update and overview of the numerous microneedle systems that utilize different activators to stimulate the release of active components from the microneedles. Further, it discusses the materials utilized for producing microneedles and the design strategies important in managing the release of drugs. An explanation of the commonly employed fabrication techniques in biomedical applications and electronics, particularly for integrated microneedle drug delivery systems, is discussed. To successfully implement microneedle technology in clinical settings, it is essential to comprehensively assess several factors, such as biocompatibility, drug stability, safety, and production cost. Finally, an in-depth review of these criteria and the difficulties and potential future direction of microneedles in delivering drugs and monitoring diseases is explored.

The utilization of polyoxometalate-based materials is largely dictated by their redox properties. Detailed understanding of the thermodynamic and kinetic efficiency of charge transfer is therefore essential to the development of polyoxometalate-based systems for target applications. Toward this end, we report electrochemical studies of a series of heteroatom-doped Keggin-type polyoxotungstate clusters [PW₁₂O₄₀]^3- (PW ₁₂ ), [VW₁₂O₄₀]^3- (V _in W ₁₂ ), [P(VW₁₁)O₄₀]^4- (PV _out W ₁₁ ), and [V(VW₁₁)O₄₀]^4- (V _in V _out W ₁₁ ) to elucidate the role of the identity and spatial location of heteroatoms and overall cluster charge on the rate constants of electron transfer and redox reaction entropies. Electrochemical analyses of the polyoxotungstates reveal that the kinetics of electron transfer for W-based redox processes change as a function of the redox activity of the heteroatom, whereas the spatial location of the heteroatom dopant does not significantly impact the electrokinetics. Variable temperature cyclic voltammetry measurements in organic solutions containing noncoordinating electrolyte ions establish that redox reaction entropies are primarily dictated by the overall charge of the clusters. Specifically, the redox entropy exhibits a good linear relationship with the dielectric continuum function Z _ox ² - Z _red ² (Z _ox = charge of oxidized species, Z _red = charge of reduced species). Finally, our experimental data do not show a prominent correlation between the kinetics of electron transfer and redox entropy, implying that the charge-transfer kinetics are not solely governed by structural reorganization. Taken together, these results highlight how structural and electronic parameters can influence the kinetics and thermodynamics of charge transfer in polyoxotungstates and provide insights into the design of polyoxometalate compounds with target redox properties.

Polymer-dispersed liquid crystals (PDLCs) stand at the intersection of polymer science and liquid crystal technology, offering a unique blend of optical versatility and mechanical durability. These composite materials are composed of droplets of liquid crystals interspersed in a matrix of polymeric materials, harnessing the optical properties of liquid crystals while benefiting from the structural integrity of polymers. The responsiveness of LCs combined with the mechanical rigidity of polymers make polymer/LC composites-where the polymer network or matrix is used to stabilize and modify the LC phase-extremely important for scientists developing novel adaptive optical devices. PDLCs have garnered significant attention due to their ability to modulate light transmission properties, making them ideal candidates for applications ranging from smart windows and displays to light shutters and privacy filters. The incorporation of different ferroelectric, thermoelectric, magnetic, and ferromagnetic nanoparticles, quantum dots, nanorods, and a variety of dyes in the PDLC matrix has gained momentum over a span of few decades, as it lowers the otherwise-required high operating voltage and reduces the electro-optical response time of these devices. Due to better contrast in the transmittance of these materials in the field-off and on states, they find extensively wide application in a variety of photonic applications, viz., optical shutters and smart windows, photorefractives, modern displays, microlens arrays encompassing polymer-gravel lenses, and many other. Since the functional parameters of these devices embrace the thermophysical attributes of PDLC networks, it therefore becomes necessary to perform a detailed analysis of the properties of PDLCs and their ameliorations upon the addition of different dopants. This Review aims to review the recent advances in PDLCs and their enrichment in terms of their performance parameters upon the addition of a variety of dopants, as well as the improvement of different photonic applications owing to superior parametric implementation of these networks.

Two-dimensional lead iodide perovskites have attracted significant attention for their potential applications in optoelectronic and photonic devices due to their tunable excitonic properties. The choice of organic spacer cations significantly influences the light emission and exciton transport properties of these materials, which are vital for their device performance. In this Perspective, we discuss the impact of spacer cations on lattice dynamics and exciton-phonon coupling, focusing on three representative 2D lead iodide perovskites that exhibit distinct types of structural distortions. Minimizing structural distortions, such as dynamic out-of-plane octahedral tilting and lone pair distortion, appears to be essential for achieving narrow photoluminescence (PL) emission peaks, high PL quantum yields, and rapid exciton diffusion by suppressing exciton-phonon coupling, as demonstrated in 2D perovskites based on phenylethylammonium cation or its derivatives. We propose that designing spacer cations with enhanced intermolecular interactions and denser packing, combined with the close packing of inorganic ions to minimize the motions of both organic and inorganic lattices, would be the ideal scenario for yielding the most favorable optoelectronic properties in these materials.

Topological quantum materials hold great promise for future technological applications. Their unique electronic properties, such as protected surface states and exotic quasi-particles, offer opportunities for designing novel electronic and spintronics devices and allow quantum information processing. The origin of the interplay between various electronic orders in topological quantum materials, such as superconductivity and magnetism, remains unclear, particularly whether these electronic orders cooperate, compete, or simply coexist. Since the 2000s, the combination of topology and matter has sparked a tremendous surge of interest among theoreticians and experimentalists alike. Novel theoretical descriptions and predictions as well as complex experimental setups confirming or refuting these theories continuously appear in renowned journals. This review aims to provide conceptual tools to understand the fundamental concepts of this ever-growing field. Superconductivity and its historical development will serve as a second pillar alongside topological materials. While the main focus of this review is topological materials such as topological insulators and semimetals, topological superconductors will be explained phenomenologically.

Ionic gels (IGs), ionic liquids (ILs) dispersed in polymers, exhibit extremely low vapor pressure, electrochemical and thermal stability, and excellent mechanical characteristics; therefore, they are used for fabricating stretchable sensors, electrochemical transistors, and energy storage devices. Although such characteristics are promising for flexible and stretchable electronics, the mechanical stress-induced ruptured covalent bonds forming polymer networks cannot recover owing to the irreversible interaction between the bonds. Physical cross-linking via noncovalent bonds enables the interaction of polymers and ILs to form supramolecular IGs (SIGs), which exhibit favorable characteristics for wearable devices that conventional IGs with noncovalent bonds cannot achieve. Herein, we review recent material designs and interactions used for fabricating SIGs, such as ionic interactions and hydrogen bonding. We present SIG characteristics achieved via the interaction of polymers and ILs, such as extreme toughness, self-healing capability, and self-adhesion favorable for human body sensors. We conclude this Perspective by discussing the potential of SIGs as a power source for implants, wearable devices, and environmental sensing applications.

The surge of flexible, biointegrated electronics has inspired continued research efforts in designing and developing chip-less and wireless devices as soft and mechanically compliant interfaces to the living systems. In recent years, innovations in materials, devices, and systems have been reported to address challenges surrounding this topic to empower their reliable operation for monitoring physiological signals. This perspective provides a brief overview of recent works reporting various chip-less electronics for sensing and actuation in diverse application scenarios. We summarize wireless signal/data/power transmission strategies, key considerations in materials design and selection, as well as successful demonstrations of sensors and actuators in wearable and implantable forms. The final section provides an outlook to the future direction down the road for performance improvement and optimization. These versatile, inexpensive, and low-power device concepts can serve as alternative strategies to existing digital wireless electronics, which will find broad applications as bidirectional biointerfaces in basic biomedical research and clinical practices.

Soft materials play a pivotal role in the efficacy of stretchable electronics and soft robotics, and the interface between the soft devices and rigid counterparts is especially crucial to the overall performance. Herein, we develop polyimide-polydimethylsiloxane (PI-PDMS) copolymers that, in various ratios, combine on a molecular level to give a series of chemically similar materials with an extremely wide Young's modulus range starting from soft 2 MPa and transitioning to rigid polymers with up to 1500 MPa. Of particular significance is the copolymers' capacity to prepare seamless stiffness gradients, as evidenced by strain distribution analyses of gradient materials, due to them being unified on a molecular level. The copolymers and gradient materials were successfully used as substrates for stretchable thin-film conductors and tested as dielectric elastomer actuators, demonstrating their potential application as enabling components in stretchable electronics and soft robots.

The oxygen evolution reaction (OER) is a critical process in various sustainable energy technologies. Despite substantial progress in catalyst development, the practical application of OER catalysts remains hindered by the ongoing challenge of balancing high catalytic activity with long-term stability. We explore the inverse trends often observed between activity and stability, drawing on key insights from both experimental and theoretical studies. Special focus is placed on the performance of different electrodes and their interaction with acidic and alkaline media across a range of electrochemical conditions. This Perspective integrates recent advancements to present a thorough framework for understanding the mechanisms underlying the activity-stability relationship, offering strategies for the rational design of next-generation OER catalysts that successfully meet the dual demands of activity and durability.

LiNi_0.5Mn_1.5O₄ (LNMO), with its high operating voltage, is a favorable cathode material for lithium-ion batteries. However, Ni and Mn dissolution and the associated low cycle life limit their widespread adoption. In this work, we investigate titanium doping as a strategy to mitigate Mn and Ni dissolution from LNMO electrodes. We demonstrate bulk doping of Ti in LNMO up to nominal compositions of x = 0.15 in LiNi_0.5Mn_1.5-x Ti _x O₄. Electrochemical characterization shows that titanium doping enhances the cycle life in LNMO-based half- and full cells with a negligible decrease in capacity or rate capability. Half-cells with LiNi_0.5Mn_1.35Ti_0.15O₄ cathodes and lithium anodes exhibited a capacity retention of 90% after 300 cycles at 1C. Li₄Ti₅O₁₂/LiNi_0.5Mn_1.35Ti_0.15O₄ full cells with Li₄Ti₅O₁₂ anodes cycled at 1C rate to 100% depth of discharge retained ∼73% of the original capacity at the end of 1000 cycles. Our work shows that cathode modification strategies could still be used for enhancing the electrochemical performance of high-voltage cathodes, while using conventional Li-ion battery electrolytes. Improving the cathode stability in conjunction with electrolyte modification could enable the development of practical high-voltage Li-ion batteries.