Chemical Reviews最新文献

As lithium-ion batteries approach their theoretical capacity limits, lithium metal batteries (LMBs) have emerged as promising candidates for next-generation energy storage, offering substantially higher energy densities. However, their practical deployment remains limited by several interrelated challenges including lithium dendrite growth, parasitic side reactions, unstable solid electrolyte interphases (SEI), and poor cycling stability. While recent advances in electrolyte design, anode architecture, and interfacial engineering have significantly improved electrochemical performance, the thermal stability and safety of LMBs, particularly at the interface and electrode levels, still require extensive investigation. This review provides a comprehensive mechanistic analysis of thermal instability in LMBs, spanning material degradation, interfacial decomposition, and cell-level thermal behavior. We critically examine the roles of lithium metal, liquid- and solid-state electrolytes, and diverse cathode chemistries (e.g., layered oxides, sulfur) in triggering exothermic reaction pathways, gas evolution, and thermal runaway. The complex coupling among electrode–electrolyte interactions, interphase chemistry, electrochemo-mechanics, morphological evolution, and thermal instability across emerging LMB chemistries is highlighted. By identifying dominant thermal instability mechanisms and key knowledge gaps, this review establishes a mechanistic foundation for designing thermally resilient LMBs and outlines future directions for advancing safety in high-energy battery systems.

A material tears, peels, and breaks by growing a crack. In a zone around the crack front, atoms undergo an irreversible process of breaking─and possibly reforming─bonds. Trailing behind the crack front are two layers of scars. Outside the irreversible zone and scars, atoms undergo the reversible process of elasticity. The irreversible zone is considered localized if it is small relative to the body. The idealization of localized irreversibility leads to a thermodynamic framework centered on the energy release rate. This crack driving force is defined using an ideal body in which a crack is stationary and deformation is elastic, and is applied to a real body in which a crack grows by an irreversible process. The irreversible zone scales with a material length: the fractocohesive length. We review recent advances in the development of crack-resistant elastomers and hydrogels as well as polymer networks reinforced by hard particles, fibers, or fabrics, subject to monotonic, cyclic, and static loading. Emphasis is placed on how molecular features, such as strand length, entanglements, noncovalent bonds, and chemical reactions, govern crack resistance. Design principles are highlighted that reconcile high toughness with low hysteresis through stress deconcentration. This review traces crack resistance to molecular origins, providing a foundation for designing next-generation crack-resistant materials.

This extensive review highlights the central role of classical molecular simulation in advancing hydrogen (H₂) technologies. As the transition to a sustainable energy landscape is urgently needed, the optimization of H₂ processes, spanning production, purification, transportation, storage, safety, and utilization is essential. To this end, accurate prediction of thermodynamic, transport, structural, and interfacial properties is important for overcoming engineering challenges across the entire H₂ value chain. Experimental measurements, despite being the traditional way of obtaining these properties, can be limited by the distinctive nature of H₂, harsh operating conditions, safety constraints, and extensive parameter spaces. Free from such limitations, classical molecular simulations, in the general frameworks of Monte Carlo and Molecular Dynamics, provide an optimal balance between computational efficiency and accuracy, bridging the gap between quantum mechanical calculations and macro-scale modeling. This review also systematically covers molecular simulation methods and force fields for computing key properties of H₂ systems, such as phase and adsorption equilibria and transport coefficients. Beyond property prediction, we explore how molecular simulation reveals fundamental mechanisms governing hydrate formation and dissociation, membrane permeations, and H₂ embrittlement. When possible, data from multiple sources are compared and critically assessed, while effort is put on evaluating the force fields used and methodological approaches followed in the literature. Finally, this review aims at identifying research gaps and future opportunities, emphasizing emerging approaches, such as molecular simulation in the era of artificial intelligence.

Ionogels, an emerging branch of gels, are polymer networks swollen with ionic liquids. Ionogels are nonvolatile and possess ionic conductivity as well as high thermal and electrochemical stability. These fascinating features make ionogels extremely attractive in many fields, such as wearable and flexible electronics, energy storage devices, and sensors. Yet, ionogels usually suffer from poor mechanical properties, which severely limits their applications. To solve this problem, a lot of effort has been devoted to improving ionogels. Here, we present a review mainly focusing on the toughening mechanisms of ionogels, given the critical role of mechanical behaviors in their applications. Meanwhile, the physicochemical properties, synthetic strategies, patterning methods, and applications of ionogels are considered. We hope this review will not only inspire further research but also provide guidance for the rational design of tough ionogels, thereby broadening their potential.

Lignocellulosic films (LCFs) have garnered significant attention due to their unique combination of flexibility, functionality, cost-effectiveness, and eco-friendliness. Defined as thin, compact, and continuous sheets with a typical thickness in the range of 10–100 μm, LCFs have been used in various fields, including packaging, flexible electronics, energy storage and harvesting, sensing, water treatment, and agriculture. Based on preparation strategies and chemical compositions, LCFs can be categorized into cellulose derivative films, regenerated cellulose films, nanocellulose films, hemicellulose films, lignin-based films, and whole lignocellulosic biomass films. While previous reviews often focus on specific types of LCFs, e.g., nanocellulose films, a comprehensive review covering all categories and their recent advancements is still lacking. This review aims to address this gap by providing a thorough overview of the basic structure and chemistry of lignocellulosic biomass, preparation strategies, functionalization methods, and the broad spectrum of applications of LCFs. Additionally, it examines the environmental and economic feasibility of LCFs and identifies strategies to overcome existing challenges, offering valuable insights for advancing the field and supporting future innovation in sustainable material science.

Colloidal particles emerge as promising building blocks for the construction of novel materials and devices owing to their tailorable morphologies, abundant species, and intriguing properties. In comparison to other assembly approaches, optical colloidal assembly relies on photophysical or photochemical interactions and allows the arrangement of particles into desired geometries on a substrate with high spatial and temporal resolution. Typically, optical colloidal assembly involves two major processes, i.e., optical manipulation for colloidal arrangement and light-triggered interparticle bonding for colloidal immobilization. In this review, we first categorize the optical manipulation techniques based on different working principles and discuss their technical features and assembly capabilities. We then provide a comprehensive overview of different colloidal bonding schemes, including van der Waals attraction, dipole–dipole interaction, biochemical linking, photopolymerization, and surface ligand bonding. Finally, we summarize the cutting-edge applications of assembled colloidal structures and end with our vision for the existing challenges and future development in this field.

Extended reality (XR) is an emerging field that connects the physical and digital worlds, enabling communication that transcends time and space. Commercial XR devices have been developed to support such experiences, but they are limited to specific sensations, mainly vibrational cues. Furthermore, these devices are realized mainly in rigid form factors, requiring external controllers or equipment, which hinders intuitive interaction and causes a mismatch with natural body movements. In this regard, skin-integrated human–machine interfaces with wearable electronics have played an important role in intuitive and immersive interaction in the XR environment, facilitating highly authentic sensory reconstruction and perception. Novel innovations in materials and structural design have enabled a wider range of sensory modalities and miniaturization, overcoming the limitations of conventional rigid XR systems. In this article, we thoroughly review human perception mechanisms to replicate hyper-realistic sensations. Then, we deal with the design and functionality for sensory feedback and input, specifically tailored for XR applications. In addition, we discuss precise system-level integration for untethered XR devices, alongside the role of artificial intelligence in real-time processing and rapid sensation conversion through predictive algorithms. Finally, we introduce promising XR applications and conclude with the challenges and prospects of future XR technologies.

Inspired by the ion transport mechanisms in biological systems, ionic technologies have emerged as a transformative field that bridges biology and electronics. Unlike electrons, ions not only transmit electrical signals but also convey chemical information and exhibit ion-specific transport behaviors. At the center of iontronic devices lie ion channels, highly selective and efficient structures that control ion transport. These ion channels, whether biological nanopores or artificial nanofluidic channels, fundamentally determine the properties of the devices. Therefore, understanding, engineering, and integrating versatile ion channels into artificial systems are critical to advancing the field. This Review provides a comprehensive overview of iontronic devices and systems, mainly covering advances after 2010, beginning with the principles of ion transport in both biological and artificial ion channels. We then examine fabrications and characterizations, with a focus on how material and structural design influence ionic properties. Device architectures are summarized and compared across multiple dimensions and scales. We highlight emerging applications in bioiontronics, neuromorphic computing, energy harvesting, water treatments, and environmental sustainability. Despite significant advancements, we propose that challenges remain in achieving the desired ion selectivity, efficient ionic signal transduction, and seamless integration of iontronics with electronics and biology.

Catalytic technology has been extensively utilized for the removal of atmospheric pollutants. Nevertheless, the intricate nature of gaseous pollutant compositions and the fluctuations in operating conditions often lead to catalyst deactivation. This review comprehensively summarizes the deactivation phenomena of catalysts during the catalytic elimination of various pollutants, including nitrogen oxides (NO_x), volatile organic compounds (VOCs), hydrocarbons (HCs), soot, and non-CO₂ greenhouse gases (CH₄, N₂O, fluorinated gases). An in-depth exploration of the deactivation mechanisms is conducted, with a focus on the potential compensatory and aggravating effects among poisons under complex operating conditions. Furthermore, effective strategies for fabricating poisoning-resistant catalysts are discussed. For instance, the incorporation of sacrificial sites is proposed as a viable approach to alleviate catalyst poisoning. The sensor system and the model for catalyst deactivation are also presented. Regarding deactivated catalysts, this review delineates effective regeneration methods. It presents a novel descriptor for selecting detoxifying agents based on acid dissociation constants and a strategy for masking intractable poisons. Finally, this review emphasizes the significance of appropriate catalyst evaluation methods in accurately gauging a catalyst’s genuine resistance to deactivation. It also highlights that rational catalyst evaluation methodologies, coupled with artificial intelligence-assisted catalyst design, hold great potential for extending catalyst lifespan and enhancing the efficient management of pollutants.