Chemical Society Reviews最新文献

The growing global energy demand necessitates the development of renewable energy solutions to mitigate greenhouse gas emissions and air pollution. To efficiently utilize renewable yet intermittent energy sources such as solar and wind power, there is a critical need for large-scale energy storage systems (EES) with high electrochemical performance. While lithium-ion batteries (LIBs) have been successfully used for EES, the surging demand and price, coupled with limited supply of crucial metals like lithium and cobalt, raised concerns about future sustainability. In this context, potassium-ion batteries (PIBs) have emerged as promising alternatives to commercial LIBs. Leveraging the low cost of potassium resources, abundant natural reserves, and the similar chemical properties of lithium and potassium, PIBs exhibit excellent potassium ion transport kinetics in electrolytes. This review starts from the fundamental principles and structural regulation of PIBs, offering a comprehensive overview of their current research status. It covers cathode materials, anode materials, electrolytes, binders, and separators, combining insights from full battery performance, degradation mechanisms, in situ/ex situ characterization, and theoretical calculations. We anticipate that this review will inspire greater interest in the development of high-efficiency PIBs and pave the way for their future commercial applications.

Two-dimensional (2D) materials, known for their distinctive electronic, mechanical, and thermal properties, have attracted considerable attention. The precise atomic-scale synthesis of 2D materials opens up new frontiers in nanotechnology, presenting novel opportunities for material design and property control but remains challenging due to the high expense of single-crystal solid metal catalysts. Liquid metals, with their fluidity, ductility, dynamic surface, and isotropy, have significantly enhanced the catalytic processes crucial for synthesizing 2D materials, including decomposition, diffusion, and nucleation, thus presenting an unprecedented precise control over material structures and properties. Besides, the emergence of liquid alloy makes the creation of diverse heterostructures possible, offering a new dimension for atomic engineering. Significant achievements have been made in this field encompassing defect-free preparation, large-area self-aligned array, phase engineering, heterostructures, etc. This review systematically summarizes these contributions from the aspects of fundamental synthesis methods, liquid catalyst selection, resulting 2D materials, and atomic engineering. Moreover, the review sheds light on the outlook and challenges in this evolving field, providing a valuable resource for deeply understanding this field. The emergence of liquid metals has undoubtedly revolutionized the traditional nanotechnology for preparing 2D materials on solid metal catalysts, offering flexible possibilities for the advancement of next-generation electronics.

Energy storage devices with high power and energy density are in demand owing to the rapidly growing population, and lithium-ion batteries (LIBs) are promising rechargeable energy storage devices. However, there are many issues associated with the development of electrode materials with a high theoretical capacity, which need to be addressed before their commercialization. Extensive research has focused on the modification and structural design of electrode materials, which are usually expensive and sophisticated. Besides, polymer binders are pivotal components for maintaining the structural integrity and stability of electrodes in LIBs. Polyvinylidene difluoride (PVDF) is a commercial binder with superior electrochemical stability, but its poor adhesion, insufficient mechanical properties, and low electronic and ionic conductivity hinder its wide application as a high-capacity electrode material. In this review, we highlight the recent progress in developing different polymeric materials (based on natural polymers and synthetic non-conductive and electronically conductive polymers) as binders for the anodes and cathodes in LIBs. The influence of the mechanical, adhesion, and self-healing properties as well as electronic and ionic conductivity of polymers on the capacity, capacity retention, rate performance and cycling life of batteries is discussed. Firstly, we analyze the failure mechanisms of binders based on the operation principle of lithium-ion batteries, introducing two models of “interface failure” and “degradation failure”. More importantly, we propose several binder parameters applicable to most lithium-ion batteries and systematically consider and summarize the relationships between the chemical structure and properties of the binder at the molecular level. Subsequently, we select silicon and sulfur active electrode materials as examples to discuss the design principles of the binder from a molecular structure point of view. Finally, we present our perspectives on the development directions of binders for next-generation high-energy-density lithium-ion batteries. We hope that this review will guide researchers in the further design of novel efficient binders for lithium-ion batteries at the molecular level, especially for high energy density electrode materials.

Globally, 91% of plant production encounters diverse environmental stresses that adversely affect their growth, leading to severe yield losses of 50–60%. In this case, monitoring the connection between the environment and plant health can balance population demands with environmental protection and resource distribution. Fluorescent chemosensors have shown great progress in monitoring the health and environment of plants due to their high sensitivity and biocompatibility. However, to date, no comprehensive analysis and systematic summary of fluorescent chemosensors used in monitoring the correlation between plant health and their environment have been reported. Thus, herein, we summarize the current fluorescent chemosensors ranging from their design strategies to applications in monitoring plant-environment interaction processes. First, we highlight the types of fluorescent chemosensors with design strategies to resolve the bottlenecks encountered in monitoring the health and living environment of plants. In addition, the applications of fluorescent small-molecule, nano and supramolecular chemosensors in the visualization of the health and living environment of plants are discussed. Finally, the major challenges and perspectives in this field are presented. This work will provide guidance for the design of efficient fluorescent chemosensors to monitor plant health, and then promote sustainable agricultural development.

Colorimetric sensing offers instant reporting via visible signals. Versus labor-intensive and instrument-dependent detection methods, colorimetric sensors present advantages including short acquisition time, high throughput screening, low cost, portability, and a user-friendly approach. These advantages have driven substantial growth in colorimetric sensors, particularly in point-of-care (POC) diagnostics. Rapid progress in nanotechnology, materials science, microfluidics technology, biomarker discovery, digital technology, and signal pattern analysis has led to a variety of colorimetric reagents and detection mechanisms, which are fundamental to advance colorimetric sensing applications. This review first summarizes the basic components (e.g., color reagents, recognition interactions, and sampling procedures) in the design of a colorimetric sensing system. It then presents the rationale design and typical examples of POC devices, e.g., lateral flow devices, microfluidic paper-based analytical devices, and wearable sensing devices. Two highlighted colorimetric formats are discussed: combinational and activatable systems based on the sensor-array and lock-and-key mechanisms, respectively. Case discussions in colorimetric assays are organized by the analyte identities. Finally, the review presents challenges and perspectives for the design and development of colorimetric detection schemes as well as applications. The goal of this review is to provide a foundational resource for developing colorimetric systems and underscoring the colorants and mechanisms that facilitate the continuing evolution of POC sensors.

Electrochemical energy conversion and storage are playing an increasingly important role in shaping the sustainable future. Differential electrochemical mass spectrometry (DEMS) offers an operando and cost-effective tool to monitor the evolution of gaseous/volatile intermediates and products during these processes. It can deliver potential-, time-, mass- and space-resolved signals which facilitate the understanding of reaction kinetics. In this review, we show the latest developments and applications of DEMS in various energy-related electrochemical reactions from three distinct perspectives. (I) What is DEMS addresses the working principles and key components of DEMS, highlighting the new and distinct instrumental configurations for different applications. (II) How to use DEMS tackles practical matters including the electrochemical test protocols, quantification of both potential and mass signals, and error analysis. (III) Where to apply DEMS is the focus of this review, dealing with concrete examples and unique values of DEMS studies in both energy conversion applications (CO₂ reduction, water electrolysis, carbon corrosion, N-related catalysis, electrosynthesis, fuel cells, photo-electrocatalysis and beyond) and energy storage applications (Li-ion batteries and beyond, metal–air batteries, supercapacitors and flow batteries). The recent development of DEMS-hyphenated techniques and the outlook of the DEMS technique are discussed at the end. As DEMS celebrates its 40th anniversary in 2024, we hope this review can offer electrochemistry researchers a comprehensive understanding of the latest developments of DEMS and will inspire them to tackle emerging scientific questions using DEMS.

The past few decades have witnessed encouraging progress in the development of high-performance film-based fluorescent sensors (FFSs) for detecting explosives, illicit drugs, chemical warfare agents (CWAs), and hazardous volatile organic chemicals (VOCs), among others. Several FFSs have transitioned from laboratory research to real-world applications, demonstrating their practical relevance. At the heart of FFS technology lies the sensing films, which play a crucial role in determining the analytes and the resulting signals. The selection of sensing fluorophores and the fabrication strategies employed in film construction are key factors that influence the fluorescence properties, active-layer structures, and overall sensing behaviors of these films. This review examines the progress and innovations in the research field of FFSs over the past two decades, focusing on advancements in fluorophore design and active-layer structural engineering. It underscores popular sensing fluorophore scaffolds and the dynamics of excited state processes. Additionally, it delves into six distinct categories of film fabrication technologies and strategies, providing insights into their advantages and limitations. This review further addresses important considerations such as photostability and substrate effects. Concluding with an overview of the field's challenges and prospects, it sheds light on the potential for further development in this burgeoning area.

Photoelectrochemical (PEC) water splitting provides a scalable and integrated platform to harness renewable solar energy for green hydrogen production. The practical implementation of PEC systems hinges on addressing three critical challenges: enhancing energy conversion efficiency, ensuring long-term stability, and achieving economic viability. Metal–insulator–semiconductor (MIS) heterojunction photoelectrodes have gained significant attention over the last decade for their ability to efficiently segregate photogenerated carriers and mitigate corrosion-induced semiconductor degradation. This review discusses the structural composition and interfacial intricacies of MIS photoelectrodes tailored for PEC water splitting. The application of MIS heterostructures across various semiconductor light-absorbing layers, including traditional photovoltaic-grade semiconductors, metal oxides, and emerging materials, is presented first. Subsequently, this review elucidates the reaction mechanisms and respective merits of vacuum and non-vacuum deposition techniques in the fabrication of the insulator layers. In the context of the metal layers, this review extends beyond the conventional scope, not only by introducing metal-based cocatalysts, but also by exploring the latest advancements in molecular and single-atom catalysts integrated within MIS photoelectrodes. Furthermore, a systematic summary of carrier transfer mechanisms and interface design principles of MIS photoelectrodes is presented, which are pivotal for optimizing energy band alignment and enhancing solar-to-chemical conversion efficiency within the PEC system. Finally, this review explores innovative derivative configurations of MIS photoelectrodes, including back-illuminated MIS photoelectrodes, inverted MIS photoelectrodes, tandem MIS photoelectrodes, and monolithically integrated wireless MIS photoelectrodes. These novel architectures address the limitations of traditional MIS structures by effectively coupling different functional modules, minimizing optical and ohmic losses, and mitigating recombination losses.

This review focusses on the significance of fluorescent, phosphorescent labelling and tracking of extracellular vesicles (EVs) for unravelling their biology, pathophysiology, and potential diagnostic and therapeutic uses. Various labeling strategies, such as lipid membrane, surface protein, luminal, nucleic acid, radionuclide, quantum dot labels, and metal complex-based stains, are evaluated for visualizing and characterizing EVs. Direct labelling with fluorescent lipophilic dyes is simple but generally lacks specificity, while surface protein labelling offers selectivity but may affect EV-cell interactions. Luminal and nucleic acid labelling strategies have their own advantages and challenges. Each labelling approach has strengths and weaknesses, which require a suitable probe and technique based on research goals, but new tetranuclear polypyridylruthenium(II) complexes as phosphorescent probes have strong phosphorescence, selective staining, and stability. Future research should prioritize the design of novel fluorescent probes and labelling platforms that can significantly enhance the efficiency, accuracy, and specificity of EV labeling, while preserving their composition and functionality. It is crucial to reduce false positive signals and explore the potential of multimodal imaging techniques to gain comprehensive insights into EVs.

Proteins are an eminently important class of ubiquitous biomacromolecules with diverse biological functions, and numerous techniques for their detection, quantification, and localisation have been developed. Many of these methods exploit the selectivity arising from molecular recognition of proteins/antigens by immunoglobulins. The combination of surface-enhanced Raman scattering (SERS) with such “immuno”-techniques to immuno-SERS (iSERS) is the central topic of this review, which is focused on colloidal SERS nanotags, i.e., molecularly functionalised noble metal nanoparticles conjugated to antibodies, for their use in protein assays and ex vivo imaging. After contrasting the fundamental differences between label-free SERS and iSERS, including a balanced description of the advantages and drawbacks of the latter, we describe the usual workflow of iSERS experiments. Milestones in the development of the iSERS technology are summarised from a historical perspective. By highlighting selected examples from the literature, we illustrate the conceptual progress that has been achieved in the fields of iSERS-based protein assays and ex vivo imaging. Finally, we attempt to predict what is necessary to fully exploit the transformative potential of the iSERS technology by stimulating the transition from research in academic labs into applications for the benefit of our society.