Chemical Society Reviews最新文献

Traditional mass spectrometry (MS)-based proteomics aims to detect and measure protein expression on a global scale and elucidate the link between protein function and phenotypic characteristics. Although advances in MS technology have significantly broadened the scope of detectable proteomes, these methodologies primarily provide data on protein abundance and offer limited insights into their functional activities. Phenotypic traits emerge from the interplay between protein abundance and functional activity, making the accurate measurement of activity a critical but challenging task, owing to the complexity of biological systems. Furthermore, the biological function of a protein is strongly linked to its interaction with other molecules within the cellular environment. Chemical proteomics offers a complementary approach that uses a toolkit developed in chemical biology to map the molecular interactome and provide initial insights into the activities of specific target proteins. However, the value of these techniques lies not in isolation, but as part of a broader experimental workflow that includes follow-up biological investigations to validate the findings and elucidate their functional relevance. This tutorial review highlights the design principles of chemical tools and examines their applications in two key areas: (i) functional activity profiling of biomolecules and (ii) molecular proximity profiling for interactome characterization. We also discuss the importance of the experimental context in shaping data interpretation and ensuring the practical adoption of these methods by biologists. Although chemical proteomics is not a standalone solution, it represents a promising step toward next-generation omics technologies and advances our understanding of biological functions at the molecular level.

Asymmetric catalysis has emerged as a pivotal strategy in the synthesis of chiral compounds, offering significant advantages in selectivity and efficiency. In recent years, heterogeneous catalysis has become a focal point in the fields of organic synthesis and materials science due to continuous advancements in science and technology, especially the use of crystalline porous materials (CPMs) as catalysts. This review summarizes recent advances in using CPMs, such as metal–organic frameworks (MOFs), covalent organic frameworks (COFs) and zeolites, as promising supports for asymmetric catalysts. These materials provide high surface areas, tunable porosity, and the ability to host active catalytic sites, which enhance reaction rates and selectivity. In this review, we summarize the stereostructural properties of chiral CPMs to guide the future design of asymmetric heterogeneous catalysts and the study of catalytic mechanisms. Moreover, we discuss various strategies for incorporating catalytic moieties into these frameworks, including direct synthesis, post-synthesis modification and induced synthesis methods. Additionally, we highlight recent examples where CPMs have been successfully applied in asymmetric transformations, examining their mechanistic insights and the role of substrate diffusion in achieving high enantioselectivity. This review concludes with a perspective on the challenges and future directions in this rapidly evolving field, emphasizing the need for further integration of advanced artificial intelligence techniques and design principles to optimize the synthesis and catalytic performance of chiral CPMs.

The interplay between ionic environments and single-molecule charge transport represents an emerging frontier in molecular electronics, offering critical insights into nanoscale electronic behavior and its chemical underpinnings. This review examines the multifaceted influence of ions on charge transport, extending beyond the conventional paradigm of energy level alignment achieved via electrochemical gating. Key points include the modulation of tunneling barrier shapes, molecular conformations, electrode work functions, and molecule–electrode coupling, as well as the critical roles of solvent–ion interactions, pH levels, and counterion effects. Both classical and innovative experimental approaches are evaluated to provide a comprehensive understanding of how ionic environments dynamically shape molecular electronics. The integration of theoretical and experimental frameworks is also addressed, with an emphasis on developing design principles for electrolytes and junction configurations to enable precise ionic control. The review highlights the importance of ionic effects in advancing molecular electronics, from fundamental chemical insights to practical applications, and discusses their implications in device design and experimental methodologies.

Surface-enhanced Raman scattering (SERS) is a powerful analytical technique, where the creation of “hotspots” holds the key to unlocking sensitive, reproducible and reliable performance. DNA nanostructures, known for their unique predictability and exceptional programmability, have emerged as promising tools for the controllable assembly and precise regulation of SERS hotspots. In recent years, the application of DNA nanotechnology in the regulation of SERS hotspots has emerged as a research focus, but a comprehensive summary of this field is still lacking. This review begins by elucidating the mechanisms of localized surface plasmon resonance (LSPR) coupling and SERS enhancement, providing a theoretical foundation for the design principles and assembly strategies for SERS hotspots. Following this, general approaches for assembling static SERS hotspots using DNA structures of different dimensions as linkers or templates are explored. Subsequently, we delve into dynamic regulation strategies for SERS hotspots mediated by DNA structures, focusing on structural reconfiguration driven by DNA hybridization, toehold-mediated strand displacement (TMSD), and enzyme-catalyzed DNA allostery, and then summarize recent examples of DNA-mediated hotspot regulation in biosensing and bioimaging applications. Finally, we discuss future perspectives associated with the DNA-mediated precise regulation of SERS hotspots, underscoring the imperative for enhanced scalability, uniformity, and integration to pave the way for real-world applications.

Membrane-free redox flow batteries (RFBs) are promising energy-storage technologies that present an innovative solution to address the critical need for sustainable and efficient energy systems. This review provides a detailed examination of membrane-free RFBs, focusing on recent technological advances and design optimization. Moreover, it highlights the growing importance of membrane-free designs for achieving higher efficiency and scalability in energy-storage systems. These designs offer significant improvements in terms of electrolyte concentration, Coulombic efficiency, and flow management, underscoring the potential of these systems for advanced energy-storage solutions. We explore the utilization of immiscible electrolyte solvents and the engineering of laminar flow dynamics to achieve efficient electrolyte separation without traditional ion-exchange membranes. The article discusses metal-free and metal-phase aqueous/nonaqueous and nonaqueous/nonaqueous immiscible solvent-based RFBs; laminar flow-based RFBs; single-phase co-laminar flow batteries; liquid/solid membrane-free RFBs; and triphasic membrane-free RFBs, highlighting their unique design features and operational benefits, as well as their potential and challenges in energy-storage applications. Key parameters such as the coulombic efficiency, self-discharge, flow dynamics, and impedance are analyzed to provide a comprehensive understanding of the performance metrics critical for the development of next-generation membrane-free RFBs. We provide valuable references for developing membrane-free RFBs and highlight their significance, technological advancements, and implications for future energy-storage applications. In the context of global energy transitions, the research and development of membrane-free batteries will provide crucial technical support for achieving sustainable energy development.

Surface plasmons, a unique optical phenomenon arising at the interface between metals and dielectrics, have garnered significant interest across fields such as biochemistry, materials science, energy, optics, and nanotechnology. Recently, plasmonics is evolving from a focus on “classical plasmonics,” which emphasizes fundamental effects and applications, to “integrative plasmonics,” which explores the integration of plasmonics with multidisciplinary technologies. This review explores this evolution, summarizing key developments in this technological shift and offering a timely discussion on the fusion mechanisms, strategies, and applications. First, we examine the integration mechanisms of plasmons within the realm of optics, detailing how fundamental plasmonic effects give rise to optical multi-effects, such as plasmon–phonon coupling, nonlinear optical effects, electromagnetically induced transparency, chirality, nanocavity resonance, and waveguides. Next, we highlight strategies for integrating plasmons with technologies beyond optics, analyzing the processes and benefits of combining plasmonics with acoustics, electronics, and thermonics, including comprehensive plasmonic-electric-acousto-thermal integration. We then review cutting-edge applications in biochemistry (molecular diagnostics), energy (harvesting and catalysis), and informatics (photonic integrated circuits). These applications involve surface-enhanced Raman scattering (SERS), surface-enhanced infrared absorption (SEIRA), surface-enhanced fluorescence (SEF), chirality, nanotweezers, photoacoustic imaging, perovskite solar cells, photocatalysis, photothermal therapy, and triboelectric nanogenerators (TENGs). Finally, we conclude with a forward-looking perspective on the challenges and future of integrative plasmonics, considering advances in mechanisms (quantum effects, spintronics, and topology), materials (Dirac semimetals and hydrogels), technologies (machine learning, edge computing, in-sensor computing, and neuroengineering), and emerging applications (5G, 6G, virtual reality, and point-of-care testing).

Merging enzymes with light-driven photocatalysis has given rise to the burgeoning field of photoenzymatic catalysis. This approach combines the high reactivity from photoexcitation with the exceptional selectivity of biocatalysis, providing exciting opportunities to tackle challenges in enantioselective radical reactions and to access new-to-nature enzyme reactivities. This tutorial review aims to provide a comprehensive introduction to this interdisciplinary topic, catering to the growing interest from communities in asymmetric catalysis, photocatalysis, radical chemistry, enzyme engineering, and synthetic biology. We summarize the fundamental principles of utilizing light to power enzymatic reactions and different strategies exploring enantioselective photoenzymatic systems, including natural cofactor-based photoenzymatic catalysis, photocatalyst/enzyme synergistic catalysis, synthetic cofactor-based artificial photoenzymes, and cofactor-free photoenzymatic catalysis. We also discuss the challenges and prospects of enantioselective photoenzymatic catalysis in advancing sustainable asymmetric synthesis.

Cancer nanomedicines have attracted significant attention in the past several decades, and the physicochemical properties, such as the size, shape, composition, surface charge, hydrophobicity, and mechanical properties, of nanoparticles have been optimized for potent cancer therapy. Since publishing our 2020 tutorial review “Influence of nanomedicine mechanical properties on tumor targeting delivery” in Chemical Society Reviews, substantial advancements have been made in understanding the role of mechanical properties in cancer nanomedicine. Notably, in vivo transport processes that are dependent on the mechanical properties of nanomedicine, including long circulation, tumor accumulation, and deep penetration, have been extensively studied using various nano-drug delivery systems. These studies have demonstrated that leveraging these mechanical properties can significantly enhance the antitumor efficacy of nanomedicine. In this review, we categorize the advancements in the mechanical properties of cancer nanomedicine into three distinct themes: the interactions between nanoparticles with varied mechanical properties and cells (2002 – present), the impact of these properties on in vivo delivery processes (2007 – present), and the strategic use of mechanical properties to boost cancer therapy (2023 – present). We analyze how different mechanical properties of organic, inorganic, hybrid, and biological nanoparticles affect their delivery processes at the macroscopic level, i.e., in tissues, organs and cells. At the microscopic level, their biological and physical interactions with biological barriers, physiological structures, cell membranes, organelles, and other structures reveal the potential mechanism of nanoparticles’ mechanical properties in determining their antitumor efficacy. Furthermore, we address the current challenges and future prospects in the mechanical properties of cancer nanomedicine, as well as the clinical translation potential of nanoparticles with diverse mechanical characteristics.

Inspired by the extraordinary attributes displayed by nanotubes in Nature, the creation of self-assembled nano-sized hollow tubes is an area of significant and growing interest given its potential application in transmembrane ion channels, ion sensing or catalysis, among others. One of the most utilized strategies employed to build these supramolecular entities implies the stacking of discrete cyclic units. Given the intrinsic dynamicity of the forces that drive the self-assembly processes, this approach offers substantial advantages when compared to inorganic or covalent approaches, ranging from tunable pore designs to error correction, to name a few. Herein we focus on the different approaches explored to design discrete cyclic entities as building blocks for the construction of self-assembled nanotubes, as well as the analytical tools used to elucidate the resulting structures. Attending to the nature of the bond involved in the formation of the cycle, we have distinguised three main categories: covalent, non-novalent and dynamic-covalent cycles. This review thus constitutes a roadmap to build self-assembled nanotubes based on soft matter and paves the way to expand their current applications.

One-dimensional (1D) van der Waals (vdWs) heterojunctions, due to the dimensional reduction leading to 1D quantum confinement effects and interface effects of the heterojunctions, typically exhibit discrete energy levels and strong electron interactions, resulting in unique conductive and optical behaviors. Carbon nanotube (CNT)-derived 1D atomic crystal vdWs heterojunctions represent a new class of 1D vdWs heterojunctions. They leverage the excellent chemical stability, nanoscale cavities, and adjustable diameters provided by CNTs as templates, ensuring controlled synthesis and precise structural tuning. The 1D radial pathways can alter the photonic–electronic propagation characteristics. At the same time, their unique metal–semiconductor-like electronic structure creates conditions for constructing various types of heterojunctions. The CNTs and their encapsulated 1D materials can lead to synergistic enhancement in the fields of electronics, magnetism, and optics. Currently, research is concentrated on understanding the synthesis mechanisms, integration characteristics, and host–guest interactions, and the exploration of novel 1D atomic crystal vdWs heterojunctions derived from CNTs. This review is focused on the latest progress made in 1D vdWs heterojunctions using CNTs as growth templates, emphasizing the construction methods, selection criteria, and the unique properties and applications arising from these complex interfacial electronic or phonon interactions. We also propose several future directions for the development of CNT-derived 1D atomic crystal vdWs heterojunctions. This review aims to enhance the understanding of their synthesis mechanisms and fundamental properties, broaden the range of available materials, and explore new and broader applications.