Accounts of Chemical Research最新文献

ConspectusTwo-dimensional (2D) organic-inorganic hybrid perovskites provide a stable alternative to three-dimensional (3D) absorbers, which often suffer from sensitivity to moisture and light. However, the traditional 2D perovskite architecture functions as a "quantum-well" structure, where insulating organic cations form dielectric barriers that restrict both light absorption and charge transport. The research described in this account focuses on transforming these passive organic spacers into active electronic components. Specifically, this transformation is achieved by incorporating diynes (molecules with two adjacent triple bonds) directly into the perovskite lattice and inducing topochemical polymerization through thermal treatment, which results in the formation of a 2D perovskite that intercalates a conductive polymer between its inorganic layers.The incorporation of such a polymer brings drastic changes in the properties of these materials. For example, it can significantly reduce their bandgap by up to 1.5 eV, thereby moving absorption well into the near-IR (NIR) range. Similarly, it can also improve the conductivity of the resulting material by up to 3 orders of magnitude while also enhancing their hydrophobicity and overall stability.In this Account, we describe the synthesis and characterization of these hybrid materials, highlighting how the inorganic lattice preorganizes diacetylene ligands to facilitate solid-state reactivity. Further, we discuss the impact of oxidative doping, showing that the incorporation of stable organic radicals in the polymers enhances electrical conductivity and the material's absorption. We further establish the versatility of this strategy by expanding the library of diynes and halides, confirming that this approach is a robust and reproducible method for modifying the optoelectronic properties of various 2D perovskite scaffolds.Beyond fundamental material design, we discuss the application of these systems in high-performance optoelectronic devices, specifically air-processed NIR photodetectors. For instance, devices utilizing one of these polymerized 2D-perovskites exhibit remarkable responsivities on par with state-of-the-art devices. Ultimately, this account argues that the integration of conjugated polymers represents a paradigm shift for 2D perovskites, successfully transforming the organic spacer from a passive dielectric barrier into an electronically active component, thereby opening the door to new and exciting properties and applications.

Electrochemical technologies represent a transformative frontier for environmental remediation, offering unparalleled advantages such as precise redox control, seamless integration with renewable energy, and chemical-free operation. However, their practical implementation in water and wastewater treatment remains constrained by inefficient mass transport, poor utilization of catalytic sites under dilute conditions, and persistent challenges in energy consumption and overall system sustainability. These limitations are particularly pronounced when treating trace contaminants or pursuing selective transformation pathways. In this Account, we summarize our recent efforts to overcome these hurdles through the development of single atom-based electrified membrane (SAEM). By integrating atomically dispersed catalytic sites into flow-through and electrically conductive membrane architectures, we have successfully coupled atomic-level active-site engineering with device-level transport intensification.

We first outline the construction principles of SAEM, highlighting how coordination environment, defect engineering, and membrane architecture collectively govern catalytic stability and site accessibility. We then examine how flow-through operation fundamentally alters transport regimes by suppressing diffusion limitations that dominate conventional flow-by and batch electrochemical systems. Building on these concepts, we discuss representative reaction systems in which SAEM exhibit clear advantages, including peroxymonosulfate activation for micropollutant degradation, in situ production of reactive oxygen species from oxygen reduction reaction for wastewater treatment, and electrocatalytic nitrate reduction for nitrogen transformation. Finally, we assess the stability, scalability, and sustainability of SAEM from a system-level perspective. Rather than focusing solely on catalytic metrics, we emphasize circularity and life-cycle considerations. This analysis underscores that the long-term viability of this platform depends on its performance as a durable, modular, and resource-efficient device within realistic treatment infrastructure.

Overall, this Account positions SAEM as a platform for integrating catalysis, separation, and environmental sustainability withinelectrochemistry, offering guiding principles for the development of advanced electrochemical technologies that are both scientifically rigorous and practically relevant.

Biomolecular condensates are membrane-less organelles formed via liquid–liquid phase separation (LLPS) in cells, which play crucial roles in organizing biochemical reactions, regulating gene expression, and responding to environmental stimuli. These dynamic membrane-less organelles, such as stress granules and nucleoli, could concentrate specific proteins and nucleic acids for spatiotemporally controlling cellular processes. The engineering of synthetic condensates is beneficial for understanding condensates formation, simulating cellular behavior, and exploration of biological pathologies.

Nucleic acid, as an important component of biomolecular condensates in cells, offers a unique platform to engineer synthetic condensates due to its programmability and precise and predictable Watson–Crick base pairing. The nucleic acid-based condensates were assembled through multivalent forces among nucleic acids or nucleic acid-peptide complexes. By designing and modifying nucleic acid sequences, the interaction forces could be regulated with external stimuli to control the formation and decomposition of nucleic acid-based condensates for various fields application. Our group has constructed various nucleic acid-based biomolecular condensates and applied them in biosensing and cellular regulation. We designed CUG repeats-based condensates for improving fluorescent RNA aptamer properties (enzymatic degradation resistance, thermal stability, photostability, and binding affinity to fluorophores) and detecting in vitro and intracellular biomolecules (adenosylmethionine and tetracycline), as well as target cells with overexpressed epithelial cell adhesion molecules. In addition, we leveraged the strong Watson–Crick base pairing ability to recruit the intracellular target RNA into condensates for cellular regulation.

In this Account, we give an overview of nucleic acid-based biomolecular condensates. We first discuss the intermolecular interactions and forces involved in the formation of nucleic acid-based biomolecular condensates. Subsequently, we summarize recent research about nucleic acid-based condensates and their applications in the fields of biological imaging and biosensing, cell simulation, cellular regulation, and drug delivery. Finally, we outline the current challenges and future opportunities of nucleic acid-based biomolecular condensates. We hope that this Account will afford significant inspiration in the design of nucleic acid-based condensates and the applications in cell biology and biomedicines.