Dynamic regulation of interfacial adhesion in biomedical hydrogels
Adhesive hydrogels represent a transformative technology in biomedicine due to their biocompatibility and multifunctionality. While extensive research has focused on improving their adhesion strength, the pursuit of long-term interfacial stability reveals a core conflict: strong adhesion often comes at the expense of easy removal. Dynamically regulating hydrogel adhesion is thus key to personalized medicine, allowing adaptation to complex clinical needs. Designing such systems demands a multifaceted approach that considers the physiological environment, medical requirements, stimulus-induced interfacial rearrangements, and mechanics-driven microstructure reconstruction. The dynamic regulation of hydrogel adhesion is more than a functional upgrade; it represents a paradigm shift for smart materials, from "static design" to "dynamic interaction". This review first introduces the mechanisms of hydrogel adhesion. It then provides an in-depth analysis of strategies for dynamically regulating adhesion at the tissue-hydrogel interface and explores the latest progress and application potential in biomedicine.
Neuromorphic iontronic devices based on soft ionic conductors
The human brain efficiently processes external information using ions as information carriers, inspiring the development of ionic brain-like intelligence. Central to such systems are neuromorphic iontronic devices (NIDs), including artificial axons, synapses, and neurons, which employ ions as charge carriers. Recently, NIDs based on soft ionic conductors (SICs), such as ionic hydrogels, ionogels, and ionic elastomers, have attracted growing attention due to their ionic compatibility, flexibility, biocompatibility, and facile fabrication and integration, making them promising candidates for next-generation neuromorphic technologies. Despite their potential, research remains in its infancy, with key challenges in elucidating fundamental mechanisms, establishing design principles, and realizing practical applications. To address these issues and guide future research, this review first introduces the functional roles and electrical signalling of axons, synapses, and neurons, thereby defining the performance requirements for NIDs. It then summarizes means for controlling ion transport in SICs and discusses feasible approaches for constructing SIC-based NIDs, including structural and interfacial engineering, device architectures, and dropletronic techniques. Finally, recent advances in SIC-based NIDs are reviewed, and their prospects in human-machine interaction and brain-like computing are discussed along with the remaining challenges.
Correction: Organoantimony: a versatile main-group platform for pnictogen-bonding and redox catalysis
Correction for 'Organoantimony: a versatile main-group platform for pnictogen-bonding and redox catalysis' by Elisa Chakraborty , , 2025, https://doi.org/10.1039/d3cs00332a.
Advances of rare earth-based catalysts for recycling CO and plastic waste
The crisis caused by the excessive use of fossil fuels-emissions of billions of tonnes of CO and the accumulation of plastic waste-is imminent. Conventional disposal technologies, such as physical storage, face risks of leakage, capacity limitations, and secondary pollution (such as microplastics). In contrast, chemical recycling, especially thermal catalytic technology, is considered a key alternative solution due to its high resource recovery potential. However, its large-scale implementation remains hindered by the absence of efficient and durable catalysts. Rare earth-based catalysts, with their unique 4f/5d electronic structure and tunable coordination environments, demonstrate significant advantages in activating inert C-C/C-H bonds, promoting CO adsorption and conversion, inhibiting coking and deactivation, and making them highly competitive for CO hydrogenation and plastic catalytic conversion. Despite rapid progress, challenges related to cost, long-term stability, and mechanistic understanding persist, impeding their industrial application. This review systematically summarises the controlled synthesis and characterisation methods of rare earth-based catalysts and thoroughly explores their applications, performance regulation mechanisms, and challenges in CO hydrogenation and plastic recycling, aiming to provide insights for designing efficient, stable, and industrially scalable rare earth catalytic systems.
Synthetic applications of electro/photochemical halogen atom transfer (XAT)-driven carbon radical chemistry
Organohalides are indispensable and widely used building blocks in organic synthesis and drug discovery due to their structural versatility, accessibility, and synthetic flexibility. The halogen atom transfer (XAT)-based strategy for generating carbon radicals from organohalides and further forming a variety of carbon-carbon and carbon-heteroatom bonds represents a powerful tool for constructing complex molecules. This approach overcomes the limitations posed by the highly negative potentials and high bond dissociation energies of organohalides, which enables the activation of inert carbon-halogen bonds under mild conditions, thus expanding the range and improving the tolerance of functional groups. In recent years, many photoredox-catalysed approaches have been reported, with advancements in energy transfer and electrochemistry leading to the development of mild methods for further functionalising organohalides and constructing complex molecules in the XAT process. This tutorial review summarises the recent advancements in research on XAT strategies for haloalkanes from the perspective of various relayed radicals such as aryl, alkyl, silyl, and boryl radicals. Detailed analysis of XAT processes of organohalides promoted by photocatalysis (energy transfer and electron donor-acceptor complex-mediated processes), electrocatalysis, and other catalytic processes is provided. Additionally, this review briefly discusses future research directions and development prospects in this field.
Recent advances in high-entropy materials for efficient alkali metal-ion batteries
Alkali metal-ion batteries (Li/Na/K, AMIBs) are considered ideal choices for grid-scale energy storage systems due to their high energy density and long cycle life. However, issues such as insufficient structural stability of electrode materials and limited ion transport dynamics in electrolytes severely restrict their large-scale commercial applications. Notably, high-entropy design strategies characterized by four core effects-the high-entropy effect, lattice distortion effect, sluggish diffusion effect, and cocktail effect-have demonstrated remarkable transformative potential by synergistically enhancing the structural stability and ion/electron transport kinetics of materials, thereby significantly improving the electrochemical performance of AMIBs. In this review, we focus on the four core effects of high-entropy materials in AMIBs, highlighting their roles in enhancing the performance of cathode/anode materials, electrolytes, electrode/electrolyte interfaces, and full cells. We comprehensively summarize the current research progress and delve into advanced characterization techniques for high-entropy materials. In addition, this review offers a detailed summary of rational structural design strategies and fundamental guiding principles for high-entropy materials in efficient AMIBs. We hope that this review will inspire greater interest in the development of high-entropy AMIBs and pave the way for their future commercial applications.
Twisted intramolecular charge transfer (TICT) based fluorescent probes and imaging agents
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.
Symmetry breaking of single-atom catalysts in heterogeneous electrocatalysis: reactivity and configuration
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-N. 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.
Electric fields at hydrophobic water interfaces: spectroscopic evidence, physical origin, and implications on reactivity
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, 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.
Single-molecule quantum tunnelling sensors
Single-molecule sensors are pivotal tools for elucidating chemical and biological phenomena. Among these, quantum tunnelling sensors occupy a unique position, due to the exceptional sensitivity of tunnelling currents to sub-ångström variations in molecular structure and electronic states. This capability enables simultaneous sub-nanometre spatial resolution and sub-millisecond temporal resolution, allowing direct observation of dynamic processes that remain concealed in ensemble measurements. This review outlines the fundamental principles of electron tunnelling through molecular junctions and highlights the development of key experimental architectures, including mechanically controllable break junctions and scanning tunnelling microscopy-based approaches. Applications in characterising molecular conformation, supramolecular binding, chemical reactivity, and biomolecular function are critically examined. Furthermore, we discuss recent methodological advances in data interpretation, particularly the integration of statistical learning and machine learning techniques to enhance signal classification and improve throughput. This review highlights the transformative potential of quantum-tunnelling-based single-molecule sensors to advance our understanding of molecular-scale mechanisms and to guide the rational design of functional molecular devices and diagnostic platforms.
Tailoring the dynamic nanocomposite hydrogels through surface-functionalized nanomaterials and interfacial crosslinking chemistry toward multifunctional biomedical and engineering applications
Dynamic nanocomposite hydrogels (DNCHs) represent a cutting-edge class of materials characterized by their tunable architecture and stimuli-responsive behavior, making them particularly well-suited for applications that require mimicking the adaptive functionality of biological systems. A wide range of chemical strategies and design methodologies have been explored to engineer their structure-property-function relationships. In this review, we present a comprehensive analysis of recent developments in DNCHs, systematically organized into six material-centric categories, including metal-, metal oxide-, carbon-, ceramic-, polymer-, and metal-organic framework (MOF)-based nanomaterials. We examine surface functionalization techniques and interfacial crosslinking mechanisms that underpin DNCH fabrication, supported by representative examples that highlight their composition, interfacial chemistry, and functional performance. We also critically evaluate current challenges and highlight key research opportunities to inform and inspire future interdisciplinary efforts. Taken together, this review presents a cohesive and forward-looking framework to support the rational design, functional implementation, and collaborative advancement of next-generation DNCHs.
Harnessing magnetic, photo, and thermal fields and their synergistic interactions for enhanced electrocatalytic oxygen evolution reaction
The oxygen evolution reaction (OER) constitutes a critical half-reaction in electrochemical water splitting and plays a central role in sustainable energy conversion systems. This review commences with an overview of the fundamental principles governing the OER, serving as the conceptual basis for understanding the influence of external physical fields on catalytic behaviour. The individual effects of magnetic, photo, and thermal fields on OER kinetics and mechanisms are systematically examined, followed by an exploration of the coupling phenomena that arise from their concurrent application. Building on these mechanistic insights, we further discuss catalyst design strategies that exploit both isolated and synergistic external field effects, as reported in recent studies. Advances in computational screening and descriptor-guided design methodologies are also reviewed. Finally, we outline critical future directions, including the optimization of performance trade-offs among activity, stability, and energy efficiency, the development of standardized evaluation protocols, and the integration of theoretical modelling to guide rational catalyst development. Collectively, this review provides a comprehensive framework for advancing OER catalysis through the strategic application of external physical fields.
Supramolecular dyes: advancing precision medicine through molecular engineering
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[]urils (CB []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.
Multi-level structural modulation enables fast lithium-ion transport in inorganic solid-state batteries
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.
Towards greener-by-design fine chemicals. Part 2: technological frontiers
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.
Recent advances in asymmetric bimetallic catalysis
Asymmetric bimetallic catalysis has emerged as a powerful and efficient approach for the development of novel enantioselective transformations. By employing two metal centers with complementary reactivity, bimetallic catalysts enable dual substrate activation, stabilize reactive intermediates, and facilitate unique transformations with high enantioselectivity. This review summarizes recent significant advances in the field, including three different reaction modes: dual metal Lewis acid catalysis, transition-metal/metal Lewis acid catalysis, and dual transition-metal catalysis. By exploring the latest breakthroughs and providing a comprehensive outlook on the promising potential of asymmetric bimetallic catalysis, we aim to inspire further progress in this rapidly evolving area and highlight future opportunities for expanding its applications.
Chirality amplification in semiconductors for advanced optoelectronics
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.
Advanced Ah-level zinc metal batteries
Aqueous zinc metal batteries (ZMBs) are emerging as promising candidates for large-scale energy storage due to their cost-effectiveness, intrinsic safety, and abundant resources. However, translating ZMBs from laboratory-scale prototypes to ampere-hour (Ah)-level practical systems remains challenging, limited by issues such as Zn dendrite growth, cathode dissolution, and the lack of scalable fabrication methods for high-mass-loading electrodes with efficient ion/electron transport. This review systematically outlines recent strategies to overcome these barriers by addressing materials, manufacturing, and cell configuration. From the material perspective, bulk and surface modifications of the Zn anode and cathode can improve electrochemical stability and capacity retention through crystal structure tuning and interface stabilization. In electrode fabrication, dry processing and hierarchical structuring have emerged as key methods to support high mass loadings while maintaining effective electron/ion transport. Further at the device level, innovations in cell configuration, like lamination, winding techniques , enable better structural integrity and electrochemical performance tailored to aqueous systems. By integrating material innovation, scalable processing, and optimized cell architecture, these developments chart a path toward practical Ah-level ZMBs. This review highlights a comprehensive framework to bridge the lab-to-market gap, guiding future efforts to realize safe, low-cost, and sustainable energy storage at scale.
Advances in oxide thermoelectric materials: strategies, applications and beyond
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.
Layered tin halide perovskites in photovoltaics
Tin-based halide perovskites are emerging as promising alternatives to traditional lead-based perovskites due to their lower bandgaps, decreased toxicity, and comparable chemical properties. These materials offer unique structural and functional benefits for optoelectronic applications and photovoltaics, particularly in their low-dimensional or layered (2D) forms. Recent advancements have improved the solar-to-electric power conversion efficiency of tin-based halide perovskites by relying on organic spacers to control crystallisation and stabilise the materials. The versatility of molecular compositions and structural tuning of layered tin halide perovskites makes them appealing for next-generation photovoltaic technologies. This review highlights the structural characteristics, synthetic methods, and properties of layered tin halide perovskites, providing a comprehensive overview and discussing future prospects for environmentally friendly perovskite photovoltaics.
Constrained carbon bonding inside fullerene cages
Carbon is an incredibly versatile element and can form bonds sp, sp, and sp hybridization, forming diverse structures, which are responsible for the vast complexity and diversity of chemistry and biology. Therefore, understanding carbon bonding is crucial for comprehending the fundamental principles of natural science. Beyond conventional chemistry, carbon bonding confined inside carbon cages can adopt unusual and seemingly unpredictable bond states. Within these spatially restricted environments, encapsulated carbon atoms can bond with multiple nonmetal atoms (, H, C, N, and O) and a variety of metal atoms (, Sc, V, Ti, and Dy), forming otherwise unstable clusters with different bonding models and oxidation states of carbon. This leads to unprecedented bonding situations, including multiple and multicenter carbon-metal bonds, covalent carbon-metal bonds, superatomic states, and pronounced donation bonds ( C → metal atoms). These bonding situations enrich the carbon bonding models beyond traditional organic chemistry. This review provides a comprehensive summary of the recent findings regarding constrained carbon bonding with varying numbers of carbon atoms inside carbon cages. It will encompass crucial aspects of this special constrained carbon bonding such as the dispersion of negative charge on the carbon cage, reduction of Coulomb repulsion, maximization of coordinated metal ions, and determination of optimal configurations for metal atoms within the carbon cages. Accordingly, new carbon bonding could be identified in carbon cages, which holds significant implications in the development of innovative carbon-based compounds. Additionally, the current challenges faced and future developments anticipated from the aspect of confined carbon bonding inside carbon cages will be discussed to provide deeper insights into the intricacies of carbon bonding. Through this comprehensive exploration, we hope to advance knowledge in this exciting area of carbon chemistry.
