Chemical Society Reviews最新文献

The global energy transition urgently demands advanced battery technologies to address current climate challenges, where molecular engineering plays a pivotal role in optimizing performance metrics such as energy density, cycling lifespan, and safety. This review systematically examines the integration of artificial intelligence (AI) into molecular discovery for next-generation battery systems, addressing both transformative potential and sustainability challenges. Firstly, multidimensional strategies for molecular representation are delineated to establish machine-readable inputs, serving as a prerequisite for AI-driven molecular discovery (Section 2). Subsequently, AI algorithms are systematically summarized, encompassing classical machine learning, deep learning, and the emerging class of large language models (Section 3). Next, the substantial potential of AI-powered predictions for key electrochemical properties is illustrated, including redox potential, viscosity, and dielectric constant (Section 4). Through paradigmatic case studies, significant applications of AI in molecular design are elucidated, spanning chemical knowledge discovery, high-throughput virtual screening, oriented molecular generation, and high-throughput experimentation (Section 5). Finally, a general conclusion and a critical perspective on current challenges and future directions are presented, emphasizing the integration of molecular databases, algorithms, computational power, and autonomous experimental platforms. AI is expected to accelerate molecular design, thereby facilitating the development of next-generation battery systems and enabling sustainable energy innovations.

Organic interface engineering has attracted increasing attention as an effective approach to tailoring electrode surfaces and improving electrocatalytic performance, while a comprehensive understanding of its underlying mechanisms remains limited. This review provides an in-depth examination of the design strategies and functional roles of organic interfaces in electrocatalysis. We categorize organic interfaces into three representative types: (i) small organic molecule-functionalized surfaces, (ii) polymer-modified electrodes, and (iii) self-assembled monolayers (SAMs). Various fabrication methods are discussed, alongside the diverse interaction mechanisms—such as covalent bonding, coordination effects, and van der Waals interactions—that govern the interface between organic components and electrode materials. We then focus on how organic interfaces contribute to catalytic enhancement by modulating local atomic arrangements, tailoring electronic structures, and constructing favorable reaction microenvironments. These interfacial modifications offer new opportunities to optimize catalytic activity, selectivity, and operational stability across a range of electrochemical transformations. Finally, we outline key challenges and future perspectives in applying organic interface strategies to practical energy conversion technologies. This review aims to bridge existing knowledge gaps and offer conceptual and methodological guidance for the rational development and design of high-performance electrocatalysts through molecular-level interface engineering.

Alkenes are an important class of organic compounds with a carbon–carbon double bond and a wide range of industrial and natural sources. The presence of π bonds provides the possibility for many forms of transformations. The direct difunctionalization of olefins can continuously introduce two identical or different groups into the olefin molecule at one time, while achieving a rapid increase in molecular complexity, and it also gives the organic compound potential or specific application value. In general, olefin difunctionalization can be achieved via three different reaction modes. Firstly, metal species can add double bonds by employing transition metals; further coupling can then be followed to complete the difunctionalization. Another intriguing approach is that radicals add to the olefins and then are quenched in diverse ways. The ability to continuously introduce diverse functional groups is the most significant feature of this platform. The third mode is that the olefin is transformed into a cationic radical or anionic radical intermediate through single-electron transfer. This strategy is less developed and more novel, but has certain limitations. Driven by the innovation of synthetic chemistry strategies, the difunctionalization of olefins, which was previously difficult to achieve, has also been gradually achieved. This review updates the latest progress in the 1,2-difunctionalization of olefins in the past five years. We aim to classify reaction mechanisms and functional group types. It should be stated that reactions with olefin double bonds to form rings are not included here.

Lanthanides play a crucial role in modern medicine and technology as well as in the metabolism of methylotrophic bacteria. In this context, the research on lanthanide-binding peptides and proteins is an active and rapidly developing field. This comprehensive and critical review focuses on the structural, thermodynamic (affinity and selectivity) and kinetic parameters governing the interaction of Ln³⁺ ions with different peptides and proteins, including both naturally occurring and de novo-designed scaffolds. It thus provides guidelines and future directions for the rational design of Ln-binding peptides and proteins with suitable features for the main applications explored to date, including luminescent sensing, magnetic resonance imaging, Ln separation and recovery and Ln-based (photo)-catalysis.

Laser ablation in liquids (LAL) has attracted widespread attention over the last decade and has gradually become an irreplaceable technique for synthesizing nanocrystals and fabricating functional nanostructures because LAL can offer effective solutions to some challenging issues in the field of nanotechnology. In the last few years, we have witnessed exciting developments in the understanding of LAL and its application for fabricating unique nanostructures, especially in the application of LAL-generated nanomaterials to biomedicine, the environment, and energy production. Following the development of LAL, we very recently developed a simple, clean, and efficient LAL-based technique, laser bubbling in liquids (LBL), to produce clean energy through hydrogen production, carbon dioxide reduction, ammonia synthesis, etc. A series of chemical reactions occur inside micro- and nanobubbles under the extreme thermodynamic state induced by a laser at normal temperature and pressure upon LBL. Compared with traditional catalytic chemical reactions, the chemical reactions that occur in the LBL process have the following characteristics. Thermodynamically, the far-from thermodynamic equilibrium state with a high temperature inside micro- and nanobubbles created by LBL provides microenvironments for chemical reactions that typically require catalyst assistance in the absence of a catalyst. In terms of kinetics, the rapid quenching of micro- and nanobubbles confined by the liquid enables accurate control of the chemical reaction and reduces the generation of byproducts. Laser production of clean energy via LBL can be expected to be a simple, green, and efficient technique on an industrial scale under normal conditions beyond chemical catalysis. This review surveys the discovery and application of LBL and provides a comprehensive understanding of laser production of clean energy and a perspective for the further development of LBL.

The apparent Gibbs energies of activation for chemical reactions that involve multiple paths in parallel and/or multiple steps in series may involve several transition states (TSs) lying close in energy. The virtual TS is a weighted average of these contributing real TSs, and the weighting factors are easily obtained from the Gibbs energies of these TSs relative to a common reactant state. Examples from organic reaction mechanisms are used to illustrate the concept and its implications for the interpretation of features of complex Hammett plots and of kinetic isotope effects (KIEs). The concept allows for a considerable simplification of the treatment of KIEs for enzymic reactions, and holds promise for the application of modern methods of computational simulation to assist in the interpretation of experimental kinetic investigations of complex mechanisms.

Phosphorus(V) stereocenters play a crucial role in the therapeutic strategies for severe diseases, including viral infections, chronic conditions, and rare genetic disorders. These diseases often involve gene-related pathologies or arise from genetic mutations that affect intracellular metabolic processes. ProTide and antisense oligonucleotide therapies are among the most effective strategies for treating such conditions, where the absolute configuration of the phosphorus center is directly linked to therapeutic efficacy. However, the development of stereodefined ProTides and PS-oligonucleotides remains a significant challenge due to the lack of efficient and scalable synthetic methodologies. This review highlights various approaches for achieving stereocontrolled synthesis of phosphorus-based ProTides and PS-oligonucleotides, including the use of stereopure precursors, chiral auxiliaries, asymmetric catalysis and enzymatic approaches. By advancing these strategies, researchers can improve the stereochemical precision of nucleotide-based therapeutics, ultimately enhancing their clinical potential. Moreover, this review examines the current methodologies utilized for the industrial-scale production of P-stereogenic ProTides and oligonucleotides.

Alzheimer's disease (AD) is a neurodegenerative disorder with a complex pathophysiology involving oxidative stress, amyloid β (Aβ) aggregation and dysregulation of metal ions, particularly copper and heme. The overproduction of reactive oxygen species (ROS) plays a crucial role in the early stages of AD, leading to lipid peroxidation, protein oxidation, nucleic acid damage and neurotransmitter oxidation. These oxidative processes are further catalysed by the accumulation of Aβ peptides, which increase ROS production, creating a self-perpetuating cycle that accelerates disease progression. This review focuses on the critical role of oxidative stress and neurotoxicity associated with heme and copper in AD pathology. Both the metal and the co-factor bind to Aβ peptides, forming complexes that amplify oxidative stress, leading to enhanced neuronal damage. The involvement of Cu/heme–Aβ complexes in redox cycling results in the production of cytotoxic hydrogen peroxide, which drives the oxidation of neurotransmitters and contributes to synaptic dysfunction. These interactions not only disrupt normal neuronal function but also intensify Aβ plaque formation, a key feature of AD progression. Understanding how heme and copper interact with Aβ, and how these interactions are influenced by important residues such as histidine, arginine and tyrosine is crucial. These amino acids play an essential role in metal coordination and in regulating the reactivity of metal/co-factor-Aβ complexes, which directly impacts neuronal health. Unveiling the interactions between Aβ peptides and Cu/heme as well as the associated oxidative reactions offers a promising direction for future research, potentially leading to strategies that mitigate oxidative stress and reduce cytotoxicity in Alzheimer's disease.

The pursuit of high-performance, sustainable, and adaptable energy storage systems stands at the forefront of addressing the ever-growing demands of our modern world. Among the most compelling frontiers in this endeavour are electrochemical technologies empowered by multi-ion carriers, which transcend the intrinsic limitations of conventional single-ion systems. By harmonizing the transport and redox behaviour of diverse cations and anions, these systems give rise to novel mechanisms of charge balance, extended electrochemical stability windows, and cooperative redox pathways. This review offers a panoramic exploration of recent advances in multi-ion carrier-enabled electrochemical energy technologies, with a particular focus on hybrid batteries, capacitors, fuel cells, and redox flow batteries. Through these case studies, we elucidate how the interplay of multiple ions governs structure–function relationships and enhances overall electrochemical performance. Central to this discussion are the underlying working principles, representative device architectures, and the latest innovations in electrode and electrolyte materials. Special attention is devoted to the way multi-ion transport phenomena unlock new electrochemical landscapes, accelerating ion kinetics, stabilizing interphases, and enabling emergent pathways unavailable to single-ion systems. We further highlight forward-looking trends in hybrid ionic configurations, such as the integration of cations, co-transport of cation–anion pairs, and the engineering of aqueous–nonaqueous hybrid systems. In closing, we provide a critical assessment of the electrochemical advantages, scalability prospects, and practical challenges that lie ahead, ranging from kinetic harmonization across multiple ions to scalable device fabrication and the mitigation of complexity-driven safety concerns. By weaving together insights from materials science, electrochemistry, and systems engineering, this review lays a foundation for the rational design of next-generation multi-ion electrochemical energy devices that promise to redefine the limits of performance and versatility.

Sodium (Na) batteries are emerging as sustainable energy storage solutions, but their performance is hindered by intrinsic challenges such as sluggish ion kinetics, dendrite formation, and interfacial incompatibility. Carbon-based materials, with their highly tunable physicochemical properties, offer versatile functionalities to address these limitations across various Na battery systems. In this review, we first explore the multi-role engineering of carbon materials in four Na battery types. Then, the correlation of carbon's structural and chemical properties (including lattice spacing, defect density, graphitic order, and pore hierarchy) with electrochemical performance was established in a functionality–performance matrix to guide material selection for specific battery designs. Building on these insights, we propose a hybrid Na battery paradigm that leverages carbon's dual capabilities: intercalation-driven Na⁺ storage for energy-oriented applications and defect-guided Na deposition for power-oriented needs. This system integrates three adaptive operation modes: standard, boost, and survival, enabling scenario-specific optimization for applications ranging from consumer electronics to grid storage and extreme environments. Finally, we identify critical challenges in carbon engineering, such as dynamic interface evolution during mode-switching and potential-driven phase transitions in hybrid systems. By bridging multi-scale carbon design with hybrid battery electrochemistry, this review provides a roadmap for developing Na batteries with broad application compatibility by carbon engineering, addressing both fundamental and technological challenges in sustainable energy storage.