Chemical Society Reviews最新文献

Solid-state lithium metal batteries (SSLMBs) are considered ideal candidates for the next-generation core technologies for development of clean energy storage and conversion systems owing to their inherent high energy density and exceptional safety. Nevertheless, the practical energy density, power characteristics, and cycling stability of SSLMBs are usually limited by sluggish charge transfer kinetics within and across solid-state components, including electrode, electrolyte, binder, and conductive additive materials. Therefore, understanding the intrinsic link between structure–charge transport–performance and improving charge transport kinetics in a heterogeneous solid system through structural modulation has become the key to comprehensively improving the electrochemical performance of SSLMBs. Herein, a unique perspective is proposed to optimize the short-range and long-range charge transport processes in SSLMBs through multi-level structural modulation at the electrode, solid electrolyte, and cell levels. We firstly summarize and evaluate the research progress in multi-level structural modulation. Then, the vital factors impacting structural regulation and regulation principles at the corresponding level are analyzed in depth. Furthermore, the extent of enhancement and limitations of various structural modulation approaches employed for charge transport are evaluated and compared. At the end, perspectives and suggestions were provided on principles for multi-level structural modulation toward fast charge transport kinetics in inorganic SSLMBs. This review will offer broadly applicable principles for the development of next-generation high-performance inorganic SSLMBs.

Precision medicine is aimed at achieving a more personalized approach tailored to individual characteristics and urgently requires the development of precise diagnostic and therapeutic methods. Small-molecule dyes play indispensable roles in medical imaging and surgery procedures, attracting significant attention regarding disease diagnosis and therapy. However, their widespread utilization for accurate tumor localization and long-term intraoperative imaging remains hindered by their inherent limitations, including tedious synthesis protocols, poor photostability, susceptibility to fluorescence quenching in physiological environments, and rapid systemic clearance. Supramolecular dyes, defined as small-molecule dye-based assemblies, usually present unique and superior photophysical properties, including tunable optical properties, enhanced photodynamic and photothermal performance, improved photostability and optimized anti-quenching capability, collectively enabling high-precision optical diagnosis and therapy. Despite remarkable progress in supramolecular dyes, a systemic review summarizing their applications in precision biomedicine remains lacking. In this review, we systematically summarize the recent advances on the development of supramolecular dyes across three key self-assembly systems: supramolecular coordination complexes (SCCs) systems, host–guest systems (including cyclodextrin, cucurbit[n]urils (CB [n]s), calixarenes and pillararenes), and enzyme instructed self-assembly (EISA) systems. Moreover, we highlight current challenges and future perspectives to accelerate their translation from fundamental research to clinical applications.

Because circularly polarized light (CPL) uniquely carries spin-selective information, chiral optoelectronics offer a powerful platform for developing high-efficiency, spin-based optical devices and driving next-generation photonic technologies. Intrinsically chiral semiconductors can absorb or emit CPL through light–matter interactions, positioning them as highly attractive active materials for advanced optoelectronics. However, their weak chiroptical activities often hinder practical implementation. To address this challenge, researchers have explored a range of strategies aimed at enhancing chiroptical performance. Recent advances in molecular design, processing techniques, and device engineering have led to significant improvements in the chiroptical properties of these materials. This review summarizes recent progress in chirality amplification strategies for semiconductors in advanced optoelectronics. Intrinsically chiral semiconductors are classified into three groups: organic semiconductors, metal–organic materials, and chiral hybrid perovskites. Furthermore, strategies for enhancing chiroptical signal output in chiral optoelectronic devices are discussed, supported by relevant theoretical frameworks. These advancements establish a solid foundation for the development of high-performance chiral optoelectronic devices, paving the way for future innovations in photonic technology.

Oxide thermoelectric materials have emerged as promising candidates for sustainable energy applications owing to their inherent thermal stability, environmental benignity, elemental abundance, and low cost. This review comprehensively summarizes the recent advances in oxide thermoelectrics, covering synthesis methodologies for bulk and thin-film oxides as well as state-of-the-art advances in thermoelectric performance. Particular emphasis is placed on multiple optimization strategies aimed at carrier-phonon decoupling in oxides (such as high entropy design, texturization, homo-structure construction, and symmetry modulation) and emerging applications based on oxide thermoelectrics (including the photothermoelectric effect, and transverse thermoelectric effect), distinguished from conventional thermoelectric energy conversion. These coupled functionalities open new avenues for multi-modal energy harvesting and intelligent device integration. Finally, we highlight critical challenges and unresolved issues that need to be addressed in future research and practical applications in oxide thermoelectrics.

Water at interfaces exhibits unique properties that differ markedly from those of bulk water. In particular, a myriad of water-interface-related enhanced reactivities including on-water catalysis and microdroplet chemistry have been documented since the 1980s but remain mechanistically unclear. This review focuses on recent advances in optical spectroscopy and imaging techniques—including fluorescence imaging, vibrational Stark spectroscopy, electrochromism, sum-frequency generation, and high-resolution Raman micro-spectroscopy—that have successfully enabled the detection of interfacial electric fields at different hydrophobic water interfaces (air, liquid and solid). We summarize how both probe-based and label-free optical spectroscopic techniques can consistently quantify the on-water electric field strengths to be on the order of tens of MV cm⁻¹, corroborated by independent non-spectroscopic techniques, such as electrokinetic and surface charge measurements. The surprisingly close agreement among these different measurements and across broad experimental systems strongly hints at the existence of strong electric fields being a general feature of water–hydrophobe interfaces. We further discuss the physical origins of the interfacial electric field with a particular emphasis on the mechanism of preferential hydroxide accumulation at hydrophobic interfaces. Finally, we examine the implications of strong interfacial electric fields for chemical kinetics, radical generation and thermodynamics, thereby making important connections to interfacial water reactivity. These insights not only contribute to our fundamental understanding of water at interfaces but also point toward new strategies for harnessing interfacial water electrostatics in biomedicine, catalysis, green chemistry, and environmental science.

Twisted Intramolecular charge transfer (TICT)-based fluorescent probes are crucial in chemical sensing due to their sensitivity and specificity. These probes undergo conformational changes upon interacting with target analytes, resulting in measurable fluorescence responses. Their environment-dependent emission characteristics make them ideal for detecting variations in solvent polarity, microviscosity, and specific chemical species. Recent advances have expanded their applications to organic optoelectronics and non-linear optics. This review discusses the design principles, mechanisms, and applications of TICT-based probes, emphasizing their role in detecting cations, anions, and neutral molecules. We describe their advantages, such as fluorescence turn-on or turn-off responses and potential for ratiometric detection, which inherently corrects for interferences. Challenges in developing these probes, including fluorescence quantum yield and photostability, are also addressed. Potential directions for future research are highlighted, including the need for improved biocompatibility and multimodal imaging capabilities, with the aim of enhancing their utility in environmental monitoring, biomedical research, and clinical diagnostics.

Single-atom catalysts (SACs) have emerged as transformative materials in heterogeneous electrocatalysis, yet their conventional symmetric coordination environments often yield suboptimal catalytic efficacy. This review systematically examines the deliberate disruption of local symmetry as a powerful design strategy to precisely tailor the electronic properties of SACs. We categorize and analyze atomic-level modulation approaches, including strain-induced lattice distortion, defect-engineered coordination tailoring, and curvature-derived interfacial fields, demonstrating how these strategies effectively break the intrinsic symmetry of motifs such as M–N₄. Our analysis reveals that such symmetry breaking redistributes electron density around the metal center, lifts orbital degeneracy, and optimizes the d-band center, leading to enhanced intermediate adsorption, accelerated reaction kinetics, and broken scaling relationships. Furthermore, these asymmetrically configured SACs exhibit improved stability through strengthened metal–support interactions. While significant progress has been made, we conclude that future efforts must address the challenges of atomic-level precision, stability under operation, and scalable synthesis to fully realize the potential of symmetry-broken SACs across various electrocatalytic applications, thereby establishing a new paradigm for the rational design of advanced electrocatalytic materials.

Over the past three decades, the pharmaceutical and agrochemical sectors have embarked on a transformative journey towards greener-by-design processes, firmly rooted in the principles of green chemistry. Building on this foundation, green engineering frameworks have expanded the focus beyond environmental concerns to encompass product quality, economic viability, and the evolving demands of modern healthcare. At the heart of this transformation is continuous and smart manufacturing due to its capacity to reduce raw material use, waste, and energy consumption. While attention has understandably centered on replacing or refining conventional batch operations, the breadth of progress is far wider. Advanced analytics and digitization, as exemplified by AI-driven modeling, are nurturing the rise of “smart factories” that autonomously optimize performance in real time. A prime illustration lies in the purification of fine chemicals, where real-time analytics and advanced process control slash solvent requirements, an acute pollution hotspot, while ensuring consistent product quality. Meanwhile, 3D printing has introduced a genuinely disruptive dimension, challenging traditional notions of scale and location through on-demand, flexible production. In this piece, we explore how these converging technological frontiers lay the groundwork for the patient-centered, eco-conscious pharmaceutical and agrochemical facilities of the future.