ACS Nano最新文献

DNA storage is expected to tackle the dilemma faced by electronic information technology for the effective storage and management of massive amounts of data in the era of big data. Efficient and reliable data retrieval is crucial for DNA storage. However, it is still challenging to actualize DNA storage with fast and accurate readout capabilities, which play a key role in the practicality and reliability of DNA storage. In this study, an integrated system was constructed using homemade microfluidic PCR and DNA magnetic beads for fast and accurate DNA storage and reading with reproducibility. The homemade microfluidic PCR and DNA magnetic beads constructed for the random access of DNA storage have the advantages of short time and low bias named MMBP. The homemade DNA magnetic beads are low cost, stable, and reproducible. The integrated DNA storage and reading system integrated by MMBP can read information not only more accurately and quickly but also at a lower sequencing depth than traditional PCR. Overall, the MMBP-based DNA information storage system (MMBP-DIS) has the advantages of reducing the cost, decreasing the random access time to 10 min, and improving the reading accuracy and sensitivity. In the future, it can be integrated with DNA electrochemical synthesis to develop a fast and accurate portable microfluidic device for DNA synthesis-preservation-reading integration.

Rapid, highly sensitive, and specific nucleic acid detection plays a crucial role in advancing point-of-care (POC) diagnostics for pathogens and viruses, cancer monitoring, and optimizing clinical treatments. Herein, leveraging the precise recognition ability of CRISPR/dCas9 and the powerful localized surface plasmon resonance (LSPR) of gold nanoparticles (AuNPs), we report the design of a dual protein corona-mediated detection platform to simultaneously fulfill rapid POC testing and single-molecule counting of nucleic acids in a one-pot and one-step manner. This system uses guide RNA as a molecular bridge to anchor dCas9 protein onto AuNPs, forming artificial protein coronas. Upon recognizing a target, the interaction between the two protein coronas on the same nucleic acid molecule triggers cross-linked aggregation of AuNPs. Then, a target as low as 100 aM can be visually detected within 30 min, making the platform particularly well-suited for rapid POC application and the screening of emerging epidemics. Additionally, the superior LSPR properties of AuNPs increase the light-scattering signal generated during target-induced aggregation, enabling the visualization of the aggregated AuNPs as diffraction-limited spots under confocal microscopy. By counting these spots, the platform achieves unprecedented detection sensitivity, identifying a target as low as 1 aM, which is equivalent to just 6 molecules in a 10 μL system, demonstrating single-molecule detection capability. This dual protein corona-mediated detection system offers exceptional promise for large-scale screening of pathogenic viruses and the early detection of cancer, particularly in applications requiring ultrahigh sensitivity at the single-molecule level.

Effectively addressing inflammation in periodontitis is challenging as conventional injectable hydrogels typically require the addition of drugs to provide sufficient anti-inflammatory effects. To overcome this limitation, we developed a multifunctional injectable hydrogel with inherent properties that antagonize the Toll-like receptor 4 and myeloid differentiation factor 2 complex (TLR4-MD2). This hydrogel allows for direct inhibition of inflammatory pathways without the need for additional drugs. We identified xylitol, caffeic acid, and citric acid as natural materials that effectively meet biological needs for anti-inflammatory and antibacterial effects as well as support bone regeneration. With this in mind, we developed a caffeic-acid-modified poly(xylitol succinate) (PXS)-based iCPC@MgO composite hydrogel and tested its potential application for periodontal regeneration. The iCPC@MgO hydrogel demonstrated rapid wet tissue adhesion and injectability, which are ascribed to incorporating catechol groups derived from caffeic acid. Intriguingly, the PXS polymer used for synthesizing the hydrogel was found to possess anti-inflammatory properties and act as an antagonist for the TLR4-MD2 complex. This hydrogel also exhibited outstanding antibacterial efficiency against Porphyromonas gingivalis and Aggregatibacter actinomycetemcomitans by stimulating antibiotic synthesis within bacteria and disrupting bacterial cell walls. In a periodontitis mouse model, the iCPC@MgO hydrogel demonstrated the therapeutic potential of reducing inflammatory factors, inhibiting dominant periodontitis-associated bacteria, and maintaining subgingival microbiota balance in addition to the regenerative effects. These properties, combined with their ecofriendly nature, firmly established the iCPC@MgO hydrogel as a highly promising option for use in periodontitis therapy as well as in tissue healing, repair, and regeneration in various other inflammatory conditions.

Flexible cilia of natural species are well-known for their capabilities to transport objects by their collective motions. Therefore, well-ordered, flexible, and stimuli-responsive artificial cilia have been developed to render similar functionalities. However, flexibility and stimuli-responsiveness of a microcilium are inherently incompatible with durability/robustness against mechanical damage, limiting the artificial cilia to applications with only gentle operating conditions. The critical (but long neglected in surface engineering) property of natural hairs is that they are rooted under the skin, allowing the regeneration of the damaged hairs from their undamaged roots (hair follicles). To integrate the functionalities of cilia and hair, we developed a fabrication strategy called stencil-assisted self-alignment of iron-laden aerosols to produce a surface termed armored regenerable cilia. This surface contains well-ordered, appropriately packed, flexible, and magneto-responsive artificial wires rooted within pores. The wall of the pore serves as the armor to protect the bottom part of the wires from mechanical damage, allowing the remaining wires to regrow when the self-alignment of iron-laden aerosols repeats. The armored regenerable cilia with functionalities such as water repellency, object manipulation, and impurity removal are expected to guide the design and fabrication of smart surfaces serving real-life applications.

Geometry-dependent plasmonic surface lattice resonances (SLRs) have garnered great interest across a range of applications, including nanolasers, sensors, photocatalysis, and nonlinear optics. However, the rational fabrication of high-quality, low-symmetry, plasmonic nanoparticle arrays over large areas remains challenging. Herein, we report a versatile strategy for the scalable fabrication of centimeter-scale plasmonic nanospindle (NS) arrays with high positional and orientational precision. Our approach combines solvent-assisted soft lithography with in situ reduction of metal precursors, enabling the cost-effective production of large-area and well-ordered NS arrays without the need of specialized equipment. The Au NS arrays exhibit superior SLRs with a ultranarrow line width of 3.9 nm and a quality factor (Q-factor) of 309. The aspect ratio and lattice geometry of the NSs can be precisely tuned by applying mechanical strain to the stretchable elastomeric template, thus, allowing us to customize the SLR performance across the near-infrared spectrum. This technique enables the precise engineering of anisotropic nanoparticle arrays in a standard chemistry laboratory, opening new possibilities for advanced plasmonic devices.

Mesenchymal stem cell (MSC) therapy has emerged as a promising alternative approach for treating acute liver failure (ALF) while confronting the shortage of low efficiency and poor engraftment within a hostile liver milieu. In this study, we establish a bioactive decellularized extracellular matrix (dECM) platform that incorporates dihydrolipoic acid (DHLA)-protected Pt nanoclusters doped with Cu (PtCu-DHLA) nanozymes and cell-laden microgels. The PtCu-DHLA nanozymes, selected for their versatility, function as antioxidant, anti-inflammatory, pro-proliferative, and pro-angiogenic agents, enhancing ALF alleviation and providing an optimal microenvironment for MSC transplantation. Additionally, a methacrylic anhydride (MA)-modified porcine liver-derived decellularized extracellular matrix (PLdECM) hydrogel (PLdECMMA) has been developed for the construction of microgels via microfluidic devices. Interferon γ (IFNγ) preconditioned MSCs encapsulated in PLdECMMA microgels exhibit enhanced immunomodulating activity and prolonged survival. PtCu-DHLA nanozymes and cell-laden microgels are codelivered by leveraging the PLdECM hydrogel for orthotopic transplantation. The transplanted dECM platform enables an efficient and successful rescue of CCl₄-induced ALF by counteracting oxidative stress, suppressing inflammatory storms, and promoting cellular regeneration. Overall, this study highlights a synergistic and reinforced strategy that combines biomimetic nanozymes with MSC therapy, offering significant potential for ALF treatment and broader applications in regenerative medicine.

Electrochemical urea synthesis via the coreduction of CO₂ and NO₃^- is a sustainable alternative to the traditional Bosch-Meiser process. However, the sluggish reaction kinetics usually result in a low efficiency. Herein, we designed a kind of quaternary PdCuCoZn medium-entropy alloy (MEA) metallene for highly selective urea electrosynthesis. The random occupation of Cu, Co, and Zn with lower electronegativity in the face-centered cubic lattice of Pd-based metallene enables abundant electron donation from transition metals to adjacent Pd atoms, leading to the formation of charge-polarized Pd^δ--Cu/Co/Zn^δ+ sites. Considering that the pivotal C- and N-intermediates, namely, *CO and *NH₂, are electrophilic and nucleophilic, respectively, such strong charge polarization would greatly benefit their respective formation and stabilization. The stable adsorption with *CO bonded to electron-rich Pd-based sites and *NH₂ bonded to electron-deficient Cu/Co/Zn-based sites is demonstrated by the combination of in situ characterizations and theoretical calculations. The proof-of-concept PdCuCoZn MEA metallene achieves a maximum urea yield rate of 1840 μg h^-1 mg^-1 and a high Faradaic efficiency of 70.2%, surpassing most of the reported state-of-the-arts. Our strategy proposed in this work is believed to enlighten the design of an effective catalyst used for multistep reactions.