ACS Nano最新文献

{"title":"Highly Efficient Intrastromal Dual-Drug Delivery by a Dissolving Bilayer Microneedle for Synergistic Therapy against Corneal Neovascularization","authors":"Zhaoliang Zhang, Hui Shi, Jinrun Chen, Ruiling Gu, Yu Li, Shuo Huai, Shan Li, Yuhan Hu, Huiling Wei, Deqing Lin, Lei Lei, Zhishu Bao, Jiaqing Wang, Xingyi Li","doi":"10.1021/acsnano.5c10610","DOIUrl":"https://doi.org/10.1021/acsnano.5c10610","url":null,"abstract":"Corneal neovascularization (CNV) is one of the major causes of vision impairment and blindness worldwide. Efficient intrastromal drug delivery of antiangiogenic agents is a significant challenge due to the presence of various ocular barriers (<i>i.e</i>., tear barrier, corneal epithelial barrier, <i>etc.</i>). Here, we report a rapidly dissolving bilayer microneedle (MN) patch, combining the anti-VEGF antibody (Ava) with an integrin-targeted anti-inflammatory drug (PF-Y-RGD), achieving synergistic therapy for CNV. Equipped with microscale needle tips, the topically applied MN patches reversibly pierce the corneal epithelium to generate microchannels, bypassing the tear/epithelial barrier and facilitating the transport of payload drugs into the stromal layer of the cornea, which significantly enhances drug bioavailability. Such MN patches exhibit biphasic drug release behavior and are also readily applicable and minimally invasive to impart good ocular tolerance. A rabbit model of CNV reveals that the combination of Ava with PF-Y-RGD in such bilayer MN patches robustly inhibits neovascularization and reduces neovascular areas and the expression of various cytokines (<i>i.e</i>., VEGF, TNF-α, IL-1β, MMP-9) in the cornea. As a strategy for efficient intrastromal drug delivery, this study promises an easy and effective way to treat CNV, which may also lead to approaches for curing various ocular disorders.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"340 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283922","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Single-Molecule Monitoring of Nucleic Acid Dynamics Using Raman Correlation Spectroscopy in Plasmonic Nanowells","authors":"Peilin Xin, Yingqi Zhao, Yuge Liang, Mulusew W. Yaltaye, Aliaksandr Hubarevich, Viktorija Pankratova, Shubo Wang, Jian-An Huang","doi":"10.1021/acsnano.5c12000","DOIUrl":"https://doi.org/10.1021/acsnano.5c12000","url":null,"abstract":"Label-free monitoring of single molecules by single-molecule surface-enhanced Raman spectroscopy (SM-SERS) in plasmonic nanopores can track the molecular dynamics and gain insight into its internal mechanism for applications including catalysis and sequencing. However, challenges including unstable plasmonic hot spot, fast molecule movement, and citrate interference hinder the SM-SERS data analysis and biomedical applications. In this study, we report a new SM-SERS method by sticking a single gold nanoparticle in a gold nanowell in air to generate a fixed plasmonic gap-mode hot spot on the particle surface for continuous single-molecule readout and long-term monitoring of DNA diffusion. The unlimited resident time of the DNA in the hot spot revealed unidirectional and back-and-forth diffusion patterns of different DNAs at single-base resolution depending on their sequences as well as cooccupation of the hot spot by citrate and DNA. Significantly, the spatial resolution of the hot spot was found to be able to cover 2 neighboring nucleobases, 1 sugar–phosphate backbone in the DNA, and 1 citrate. By using Raman correlation spectroscopy, the diffusion times of nucleobases in the DNAs were calculated as 5–22 s depending on molecular structures, while those of citrate were 0.1–7 s. Our results were so promising for monitoring biomolecular dynamics that they could be used to investigate oligonucleotide hybridization kinetics and may set the basis for developing SM-SERS sequencing technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"108 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289368","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Defect-Driven Degradation of MXenes in Aqueous Environments and Mitigation Strategies: Insights from First-Principles","authors":"Ana-Maria Stratulat, Valentina Nesterova, Vladislav Korostelev, Majid Beidaghi, Vadym Mochalin, Konstantin Klyukin","doi":"10.1021/acsnano.5c09946","DOIUrl":"https://doi.org/10.1021/acsnano.5c09946","url":null,"abstract":"MXenes have attracted considerable attention due to their tunable surface chemistry, high electrical conductivity, and ease of solution processing, making them promising candidates for a wide array of applications. The inherent tendency of MXenes to degrade under environmental conditions constrains their compositional diversity and limits certain practical applications. Our computational study shows that degradation of defect-free Ti₃C₂T_<i>x</i> is kinetically limited, whereas common defects markedly lower the activation barriers for water attack. Using ab initio molecular dynamics simulations (AIMD) combined with thermodynamic analysis, we show that titanium vacancies V_Ti act as active sites for the protonation of subsurface carbon atoms, weakening the bonds with and accelerating the release of adjacent Ti atoms. Targeted passivation of these sites by adsorbed metal cations (e.g., Li⁺, Na⁺, K⁺, and Mg²⁺) is predicted to effectively mitigate degradation by suppressing protonation and increasing the barrier for Ti oxidation. This stabilization arises from two synergistic effects: (i) electronic structure modification driven by a strong dipole moment, which markedly shifts the work function, and (ii) steric hindrance that limits water access to reactive defect sites. We also demonstrate that carbon vacancies V_C significantly destabilize adjacent Ti atoms, lowering the energy barrier for the water attack reaction. The substitution of V_C with electronegative species such as O or N does not significantly improve the stability of Ti₃C₂T_<i>x</i>, highlighting the detrimental role of any defects in the carbon sublattice. Because V_C are typically inherited from the precursor phase and cannot be removed during postsynthesis, controlling their concentration during M_<i>n</i>+1AX_<i>n</i> phases synthesis is essential. Our thermodynamic analysis reveals that A-rich (e.g., Al-rich) synthesis conditions substantially increase the formation energy of V_C and V_N defects in a large spectrum of M_<i>n</i>+1AX_<i>n</i> phases, providing a generalizable strategy for defect suppression and improved durability of the resulting MXenes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"8 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrically Tunable Flexible Circularly Polarized Laser with Ultrahigh Asymmetry Factor","authors":"Guodan Wei, Rui Duan, Yuan Wang, Tairan Yang, Tianhua Ren, Junzi Li, Yanyan Cui, Tesen Zhang, Handong Sun","doi":"10.1021/acsnano.5c13435","DOIUrl":"https://doi.org/10.1021/acsnano.5c13435","url":null,"abstract":"Circularly polarized (CP) laser emission delivers considerable promise for future photonic applications of chiral light sources and investigation of chiral light–matter interactions. However, the low asymmetry factor (<i>g</i>_lum) and lack of effective tuning have significantly hindered the development of such chiral light sources. Herein, multicolor (blue, green, and red) flexible CP lasers are demonstrated based on dye-doped cholesteric liquid crystal (CLC) microdroplets embedded in a polydimethylsiloxane (PDMS) elastomer. The CLC microdroplets, characterized by their left- or right-handed helical superstructures, serve as chiral cavities, facilitating the realization of CP lasing. By integrating chiral coating, CP lasing with opposite handedness is further effectively separated, notably enhancing the circular polarization degree and enabling an ultrahigh asymmetry factor (<i>g</i>_lum = 1.72). Importantly, these flexible CP lasers exhibit both electrically and mechanically tunable emission, demonstrating excellent wavelength tunability. In addition, the applied electric field allows dynamic control over the laser emission intensity, enabling fully reversible on/off switching. This work represents an important step forward to the development of high-performance chiral light sources with facile tunability and offers valuable insights for future chiroptical device design.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"N-Acetylcysteine-Capped TLQP21-Containing Au Nanocages Alleviate Depression in Mice","authors":"Meng Shi, Xiangyu Li, Zhen Fan, Yi Wang, Congcong Li, Yuanmeng Ning, Yizhao Ma, Min Sun, Xiaohuan Xia, Jianzhong Du, Jialin C. Zheng","doi":"10.1021/acsnano.5c11681","DOIUrl":"https://doi.org/10.1021/acsnano.5c11681","url":null,"abstract":"Major depressive disorder (MDD) is the most prevalent neuropsychiatric disorder globally. Promising therapies for MDD are urgently needed due to the limited effectiveness, delayed efficacy, and non-negligible side effects of current treatments. Oxidative stress and neuroinflammation have been recognized as key contributors to MDD. Here, we developed an antioxidant <i>N</i>-acetylcysteine (NAC)-capped Au nanocage (TNNC) that entrapped VGF-derived peptide TLQP21 with neuro-immunomodulatory effects. Once internalized by cells suffering from oxidative stress, NAC was consumed, and TLQP21 was released from TNNC. TNNC administration alleviated MDD-like behaviors of the chronic unpredictable mild stress (CUMS)-exposed mice and effectively relieved oxidative stress in the brains. Moreover, TLQP21 in TNNC inhibits the activation, excessive synaptic pruning, and inflammatory responses of microglia through targeting the complement C1q receptor (C1qR) and complement C3a receptor 1 (C3aR1). This work provides a bioinspired strategy to target multiple pathogenic factors in one nanoparticle for the intervention of MDD and other diseases.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283923","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Two Orders of Magnitude Reduction in Computational Load Achieved by Ultrawideband Responses of an Ion-Gating Reservoir","authors":"Daiki Nishioka, Hina Kitano, Wataru Namiki, Satofumi Souma, Kazuya Terabe, Takashi Tsuchiya","doi":"10.1021/acsnano.5c06174","DOIUrl":"https://doi.org/10.1021/acsnano.5c06174","url":null,"abstract":"The rising energy demands of conventional AI systems underscore the need for efficient computing technologies, such as brain-inspired computing. Physical reservoir computing (PRC), leveraging the nonlinear dynamics of physical systems for information processing, has emerged as a promising approach for neuromorphic computing. However, current PRC systems are constrained by narrow responsive time scales and limited performance. To address these challenges, an ion-gel/graphene electric double layer (EDL) transistor-based ion-gating reservoir (IGR) was developed. This IGR achieves a highly tunable and ultrawide time-scale response through the coexistence of fast EDL dynamics at the ion-gel/graphene interface and slower molecular adsorption dynamics on the graphene surface. Consequently, the system demonstrates an exceptionally broad responsive range, from 1 MHz to 20 Hz, while maintaining a high information processing capacity and adaptability across multiple time scales. The IGR achieved deep learning (DL)-level accuracy in chaotic time series prediction tasks while reducing computational resource requirements to 1/100 of those needed by DL. Principal component analysis reveals the IGR’s superior performance stems from its high-dimensionality, driven by the ultrawideband responses of the EDL along with the ambipolar behavior of graphene. The proposed IGR represents a significant step forward in providing low-power, high-performance computing solutions, particularly for resource-constrained edge environments.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Spin-Polarized Electron Transport Promotes the Oxygen Reduction Reaction","authors":"Priscila Vensaus, Yunchang Liang, Jean-Philippe Ansermet, Jonas Fransson, Magalí Lingenfelder","doi":"10.1021/acsnano.5c14333","DOIUrl":"https://doi.org/10.1021/acsnano.5c14333","url":null,"abstract":"Oxygen evolution (OER) and oxygen reduction (ORR) reactions are central to the efficiency of electrolysis and fuel cells, involving the paramagnetic triplet ground state of oxygen and the singlet ground state of water. Here, we demonstrate that spin-polarized currents enhance the ORR activity. Using a silver-coated nickel electrode over a neodymium (Nd) magnet, we observed that ORR performance is maximized when the Ag layer is thinner than the spin diffusion length of silver─conditions under which spin alignment at the electrode–electrolyte interface is maintained. In contrast, experiments with thicker Ag layers lead to spin relaxation and diminished electrocatalytic activity. A model description of this system shows that a substantial spin polarization at the interface is accompanied by a large two-electron transfer, which satisfies conservation of angular momentum during ORR. These findings highlight the critical role of spin-selective charge transfer and offer insights into the control of reaction pathways in oxygen electrocatalysis.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"53 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Thermally Activated Negative Differential Resistance VOx Memristor with Switchable Rate and Leaky Integrate-and-Fire Spiking Dynamics","authors":"Li-Chung Shih, Zih-Siao Liao, Gennady Cherkashinin, Eszter Piros, Lambert Alff, Jen-Sue Chen","doi":"10.1021/acsnano.5c11481","DOIUrl":"https://doi.org/10.1021/acsnano.5c11481","url":null,"abstract":"Spiking neural networks (SNNs) require neuron devices that are both compact and capable of supporting continuous-time and event-based dynamics. Here, we demonstrate a VO_<i>x</i>-based threshold switching memristor (TSM) that intrinsically enables dual-mode operation, functioning as both a spiking encoder and a leaky integrate-and-fire (LIF) neuron. While such dual behavior is theoretically possible in volatile memristors, it has only been experimentally demonstrated in limited cases. It is achieved intrinsically in a single VO_<i>x</i>-based device, arising from a thermally driven insulator-to-metal transition (IMT) within the VO_<i>x</i> layer, confirmed by temperature-dependent XRD and correlated with snap-back negative differential resistance (NDR) observed in electrical measurements. Integrated into a passive circuit, the device generates high-frequency spike trains under analog input and tunable LIF responses under pulsed stimulation. The device achieves a maximum spiking frequency of 570 kHz, a time-to-first-spike (TTFS) of 1.6 μs, and energy consumption as low as 4.7 nJ per spike. These results highlight the strong coupling between structural phase dynamics and neuronal functions, positioning the VO_<i>x</i> TSM as a promising platform for scalable neuromorphic hardware with biologically realistic spiking capabilities.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"213 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Machine Learning Framework for Modeling Ensemble Properties of Atomically Disordered Materials","authors":"Zhenyao Fang, Ting-Wei Hsu, Qimin Yan","doi":"10.1021/acsnano.5c13080","DOIUrl":"https://doi.org/10.1021/acsnano.5c13080","url":null,"abstract":"Atomic disorder can strongly influence material properties such as charge transport, optical response, and catalytic activity. However, efficiently modeling these disorder effects remains challenging for first-principles methods due to the cost of sampling large configurational spaces and computing complex physical quantities. Recent advances of machine learning techniques, particularly graph neural networks (GNNs), has enabled the efficient and accurate predictions of complex material properties, offering promising tools for studying disordered systems. In this work, we present a general machine-learning-assisted computational framework that integrates equivariant GNNs with Monte Carlo simulations to compute the thermodynamic and ensemble-averaged functional properties of disordered materials. Using the surface-termination-disordered MXene monolayer Ti₃C₂T_2–<i>x</i> as a representative system, we find that electrical conductivity exhibits an emergent peak near the order–disorder phase transition temperature due to the interplay between electron scattering and doping. In contrast, optical conductivity remains largely insensitive to local atomic disorder and reflects the global surface chemical composition. These results highlight the role of atomic disorder in affecting material properties and demonstrate the potential of our approach for statistically modeling disorder effects in a wide range of materials such as high-entropy alloys and spin liquids.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"34 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Calreticulin Enhances Therapeutic Immune Responses of Dry Thermostat-Stressed Hepatocellular Carcinoma Cell Vaccine","authors":"Da Zhang, Xinyue Fu, Chenxi Zhou, Xiaohua Xing, Youshi Zheng, Yang Zhou, Xiaoyuan Zheng, Geng Chen, Jianhua Zou, Yongyi Zeng, Xiaolong Liu","doi":"10.1021/acsnano.5c07598","DOIUrl":"https://doi.org/10.1021/acsnano.5c07598","url":null,"abstract":"Despite the promise of whole tumor cell vaccines in personalized cancer immunotherapy, their limited immunogenicity and lack of danger signals hinder their clinical efficacy. Herein, we introduce a time-efficient (within 2 h) dry thermostat (DT) device-based method to prepare ^CpGRTC-vax¹⁰⁰, a therapeutic vaccine generated by treating tumor cells through DT and further decorated with cholesterol-linked CpG-ODNs, to eliminate orthotopic hepatocellular carcinoma (HCC). The DT treatment preserves tumor cell morphology integrity and antigenic activity, promotes the translocation of calreticulin to the cell surface (approximately 13-fold), upregulates HSP70 (around 3.4-fold), and induces DNA breaks while immediately inactivating tumor cells within 5 min. This approach overcomes the limitations of existing whole cell vaccines by enhancing immunogenicity and exposing pathogen-associated and damage-associated molecular patterns. These changes led to efficient tumor antigen uptake, dendritic cell activation, and increased levels of CXCL-10, Gzms-B, IL-6, and IL-12 in tumors. Consequently, the T-cell infiltration into orthotopic HCC is enhanced. Mechanistic studies reveal that NK cells, CD4⁺T cells, and activated CD8⁺T cells are recruited, alongside with reduced Tregs within the tumor. Furthermore, ^CpGRTC-vax¹⁰⁰ activates patient-derived DC-T cells, demonstrating an efficient antitumor effect in patient-derived xenograft models through adoptive transfer of activated DC-T cells. Our findings highlight the potential of physical methods in enhancing tumor cell vaccine immunogenicity and their therapeutic promise for addressing the urgent needs of HCC treatment.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"94 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}