{"title":"Linearly Programmable Oxygen-Doped MoS2 Memtransistor for Neuromorphic Computing.","authors":"Wen Deng,Yimeng Yu,Xin Yan,Lisheng Wang,Niannian Yu,Xiaobin Liao,Wen Luo,Jinsong Wu","doi":"10.1021/acsnano.5c06688","DOIUrl":"https://doi.org/10.1021/acsnano.5c06688","url":null,"abstract":"The investigation of two-dimensional material memtransistors based on surface defect dynamics modulation holds significant importance for the development of efficient artificial heterosynaptic and advanced bionic systems. Thus, reported herein is an interfacial control technology that combines inert-atmosphere thermal annealing with low-temperature ultraviolet ozone doping. Employing this method enables efficient p-type doping of MoS2 with mild and low damage, and the constructed four-terminal heterosynaptic memtransistor exhibits high switching ratio and linearly programmable memristive switching characteristics. Here, in situ observations of controlled oxygen incorporation and oxygen vacancy migration in the MoS2 channel region using electron microscopy and in situ spectroscopy reveal a valence-change mechanism dominated by dynamic ion migration. Notably, the lateral two-dimensional (2D) bottom-gate device architecture enables this heterosynaptic device to exhibit short-term and long-term synaptic plasticity and brain-inspired associative memory in response to optical and electrical stimuli with gate tunability learn. In addition, the designed hardware-level bionic visual-haptic system successfully realizes the self-denoising function of 28 × 28 pixel images and the recognition accuracy of up to 97.6%. The excellent performance of photo- and electric-heterosynaptic makes them exhibit superior capabilities in efficient neuromorphic computing, which provides a good paradigm for realizing efficient and complex neuromorphic electronics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"54 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701054","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":"Orthopedic Implant Infection Management: Prevention, Barrier Breakthrough, and Immunomodulation.","authors":"Jiafeng Yi,Zhiqiang Chen,Rui Li,Ziyin Xu,Yue Song,Qingrui Fan,Jianjun Wang,Wei Chai","doi":"10.1021/acsnano.4c17509","DOIUrl":"https://doi.org/10.1021/acsnano.4c17509","url":null,"abstract":"The widespread use of biomedical implants has led to a surge in implant-associated infections, particularly in orthopedic applications, where biofilm formation, antibiotic resistance, and immune dysregulation synergistically exacerbate therapeutic challenges, increasing patient morbidity and healthcare burdens. This review delineates the pathogenic mechanisms, especially for Staphylococcus aureus, underpinning microbial persistence in orthopedic implant infections. Key mechanisms include biofilm-mediated physical barrier formation, abscesses, invasion of the osteocyte lacuno-canalicular network, and immune evasion that shield pathogens from antimicrobial agents and host defenses. We also outline recent advancements in infection, strategies to overcome physical barriers, such as biofilms and abscesses, and interventions aimed at modulating host immune responses to enhance bacterial clearance and tissue repair. By integrating perspectives from microbiology, immunology, and biomaterials science, we advocate for a paradigm shift toward multidimensional therapeutic approaches that synergistically address infection prevention, barrier penetration, and immune regulation. Such an integrated strategy is essential for tackling this critical and growing clinical challenge in orthopedic medicine.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"20 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701403","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":"Intermolecular Interaction Adjustment for LiNO3 Solubility Promotion toward High-Performance Li||NCM811 Batteries.","authors":"Chong Xu,Shuang Liu,Sai Che,Guang Ma,Gong Cheng,Dongyuan Zhang,Junjie Fu,Ye Wang,Jiahao Yang,Yuci Tian,Yongpeng Cui,Weihua Chen,Yongfeng Li","doi":"10.1021/acsnano.5c07805","DOIUrl":"https://doi.org/10.1021/acsnano.5c07805","url":null,"abstract":"Incorporating lithium nitrate (LiNO3) as a film-forming additive into carbonate-based electrolytes presents a promising strategy to enhance the stability of high-energy-density Li||NCM811 batteries. However, the small size of Li+ and the high donor number (DN) of NO3- hinder the dissociation of LiNO3, and its limited solubility (<800 ppm) in carbonate-based electrolytes poses significant challenges for practical application. To address this issue, we propose a \"Small-Sized Carrier\" strategy that enhances the solubility of LiNO3 in carbonate solvents by modulating the intermolecular interactions within the solvent system. This approach employs vinylene carbonate (VC), a small molecule with moderate polarity, to enhance the dissolution of LiNO3 without compromising the compatibility of the electrolyte with the lithium metal anode. The introduction of the \"Small-Sized Carrier\" additive system simultaneously enhances the stability of the electrode-electrolyte interfaces and optimizes the solvation structure of the electrolyte. As a result, the electrolyte developed through this strategy demonstrates outstanding electrochemical performance, with Li||NCM811 batteries achieving a capacity retention of 83.8% after 600 cycles. This work provides an insightful approach to designing advanced electrolytes tailored to high-energy-density lithium metal batteries (LMBs).","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701384","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}
ACS NanoPub Date : 2025-07-25DOI: 10.1021/acsnano.5c04200
Benediktus Madika,Aditi Saha,Chaeyul Kang,Batzorig Buyantogtokh,Joshua Agar,Chris M Wolverton,Peter Voorhees,Peter Littlewood,Sergei Kalinin,Seungbum Hong
{"title":"Artificial Intelligence for Materials Discovery, Development, and Optimization.","authors":"Benediktus Madika,Aditi Saha,Chaeyul Kang,Batzorig Buyantogtokh,Joshua Agar,Chris M Wolverton,Peter Voorhees,Peter Littlewood,Sergei Kalinin,Seungbum Hong","doi":"10.1021/acsnano.5c04200","DOIUrl":"https://doi.org/10.1021/acsnano.5c04200","url":null,"abstract":"This review highlights the recent transformative impact of artificial intelligence (AI), machine learning (ML), and deep learning (DL) on materials science, emphasizing their applications in materials discovery, development, and optimization. AI-driven methods have revolutionized materials discovery through structure generation, property prediction, high-throughput (HT) screening, and computational design while advancing development with improved characterization and autonomous experimentation. Optimization has also benefited from AI's ability to enhance materials design and processes. The review will introduce fundamental AI and ML concepts, including supervised learning, unsupervised learning, semi-supervised learning, and reinforcement learning (RL), alongside advanced DL models such as recurrent neural networks (RNNs), convolutional neural networks (CNNs), graph neural networks (GNNs), generative models, and Transformer-based models, which are critical for analyzing complex material data sets. It also covers core topics in materials informatics, including structure-property relationships, material descriptors, quantitative structure-property relationships (QSPR), and strategies for managing missing data and small data sets. Despite these advancements, challenges such as inconsistent data quality, limited model interpretability, and a lack of standardized data-sharing frameworks persist. Future efforts will focus on improving robustness, integrating causal reasoning and physics-informed AI, and leveraging multimodal models to enhance scalability and transparency, unlocking new opportunities for more advanced materials discovery, development, and optimization. Furthermore, the integration of quantum computing with AI will enable faster and more accurate results, and ethical frameworks will ensure responsible human-AI collaboration, addressing concerns of bias, transparency, and accountability in decision-making.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"29 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701380","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}
ACS NanoPub Date : 2025-07-25DOI: 10.1021/acsnano.5c06747
Jin Ma,Yichong Cai,Sida Rong,Mengqi Zhang,Jianing Zhang,Zheng Han,Shiqi Liu,Wenyin Yang,Changkun Zhang,Feifei Zhang,Ya Ji
{"title":"Dual-Platform Single-Molecule Redox-Targeting Reaction in Neutral Anthraquinone Flow Batteries.","authors":"Jin Ma,Yichong Cai,Sida Rong,Mengqi Zhang,Jianing Zhang,Zheng Han,Shiqi Liu,Wenyin Yang,Changkun Zhang,Feifei Zhang,Ya Ji","doi":"10.1021/acsnano.5c06747","DOIUrl":"https://doi.org/10.1021/acsnano.5c06747","url":null,"abstract":"Aqueous organic redox flow batteries (AORFBs) represent a promising technology for large-scale energy storage due to their high abundance in nature, safety, cost-effectiveness, and flexibility in molecular design. However, AORFBs suffer from a low energy density and unsatisfactory stability. Herein, we report a pH-neutral and high-energy-density anthraquinone-based flow battery utilizing a redox-targeting (RT) concept. Interestingly, single-molecule redox-targeting (SMRT) reaction with two voltage plateaus is successfully designed between redox mediator (RM) anthraquinone-2,7-disulfonic acid disodium salt (2,7-AQDS) and solid material poly(2,5-dihydroxy-1,4-benzoquinone-3,6-methylene) (PDBM) harnessing proton-coupled electron transfer, combining the advantages of both SMRT and dual-RM RT systems. The neutral RT flow battery in this work exhibits impressive performance with a series of excellent results including a high volumetric capacity of 97.1 Ah L-1 (based on the volume of anolyte, 14.22 times that of blank RFB), a coulombic efficiency of 99.99%, a capacity retention of 99.9% per cycle, and solid material utilization of 92.5%. Inspiringly, operando nuclear magnetic resonance and ultraviolet-visible spectroscopy are employed to dynamically monitor the solid-liquid interface between PDBM and AQDS during battery cycling, successfully demonstrating the two reversible redox-targeting reaction processes. This work develops a neutral, energy-dense aqueous organic redox flow battery, extensively elucidating the fundamental mechanism of the dual-plateau SMRT reaction, presenting a promising solution to large-scale long-duration energy storage.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"55 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701382","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}
ACS NanoPub Date : 2025-07-24DOI: 10.1021/acsnano.5c04674
Gyeong-Ji Kim,Kyung Ho Kim,Byoungjin Lee,Munjung Han,Seunghee Rho,Seok Young Hong,Hyung Kyo Kim,Seon Joo Park,Wan Soo Yun,Yoo Min Park,Kyoung G Lee,Kyong-Cheol Ko,Oh Seok Kwon
{"title":"Multiplexed Ultrafast Photothermal Digital Polymerase Chain Reaction Based on Oligo(Phenylene-Ethynylene).","authors":"Gyeong-Ji Kim,Kyung Ho Kim,Byoungjin Lee,Munjung Han,Seunghee Rho,Seok Young Hong,Hyung Kyo Kim,Seon Joo Park,Wan Soo Yun,Yoo Min Park,Kyoung G Lee,Kyong-Cheol Ko,Oh Seok Kwon","doi":"10.1021/acsnano.5c04674","DOIUrl":"https://doi.org/10.1021/acsnano.5c04674","url":null,"abstract":"Periodontal disease results from an imbalance between bacterial complexes and the immune system. However, periodontal disease diagnosis is limited by its time-consuming nature, long processing time, and high costs. In this study, we suggest an ultrafast, highly sensitive, and multitargeted plasmonic photothermal-based digital polymerase chain reaction (dPCR) method using a novel plasmonic photothermal-based dPCR chip combined with photothermal materials and organic interfacial chemicals for periodontal disease diagnosis. This platform can detect biofilm-forming bacteria (Streptococcus mutans), red complex bacteria (Porphyromonas gingivalis), and orange complex bacteria (Campylobacter rectus and Prevotella nigrescens). The ultrafast plasmonic photothermal-based dPCR technique amplified multiple target genes over 45 cycles within 14 min, and a fluorescence scanning system measured the fluorescence intensity within 9 min. The sensitivity of detection of standard bacteria and artificial saliva containing bacteria showed a sensitivity of 101 copies/μL. Furthermore, multiplex PCR was performed with a plasmonic photothermal-based dPCR device to confirm the possibility of multiplex PCR of bacterial mixtures containing four species. This plasmonic photothermal-based dPCR platform can be utilized as a point-of-care molecular diagnostic device for the ultrafast diagnosis of diseases in real-time in various fields.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"115 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693548","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}
ACS NanoPub Date : 2025-07-24DOI: 10.1021/acsnano.5c10591
Yan Li,Wanlin Jia,Mingting Zhu,Xinru Hu,Zhen Ya,Yichen Liu,Yujin Zong,Shifang Guo,Mingxi Wan
{"title":"Focused Acoustic Vortex-Activated Dual-Stimuli Nanoplatform Synergizes with Checkpoint Blockade to Enhance Macrophage Phagocytosis and Antitumor Immunity.","authors":"Yan Li,Wanlin Jia,Mingting Zhu,Xinru Hu,Zhen Ya,Yichen Liu,Yujin Zong,Shifang Guo,Mingxi Wan","doi":"10.1021/acsnano.5c10591","DOIUrl":"https://doi.org/10.1021/acsnano.5c10591","url":null,"abstract":"Macrophage activation in tumor immunotherapy is hindered by the \"do not eat me\" evasion mechanism, mediated by the CD47-SIRPα axis. Current therapeutic strategies that solely block antiphagocytic signals show limited efficacy in solid tumors, indicating the urgent need to simultaneously enhance \"eat me\" signals. To this end, we developed a focused acoustic vortex (FAV)-triggered dual-stimuli-responsive nanoplatform to enhance macrophage phagocytosis. This nanoplatform consists of a liposome coloaded with Cas9/sgRNA complexes and the sonosensitizer chlorin e6 (Ce6), enabling a FAV-triggered activation cascade. Upon FAV exposure, this system facilitates (1) enhanced cellular uptake by increasing membrane permeability through cavitation; (2) activation of Ce6 to generate reactive oxygen species, inducing calreticulin exposure to enhance \"eat-me\" signals; and (3) disruption of endosomes/lysosomes to release the Cas9/sgRNA complexes for CD47-specific knockout. This strategy enhanced macrophage phagocytosis of tumor cells, promoted M2-to-M1 macrophage polarization, and activated T-cell-mediated immune responses, resulting in significant antitumor efficacy in the 4T1-tumor-bearing mouse model. Programmed death-ligand 1 (PD-L1) checkpoint blockade following nanoplatform activation amplified systemic immune responses, resulting in 90% inhibition of primary and 80% inhibition of distant 4T1 tumors, and long-term immune memory. This study presents a strategy for precision immunotherapy through spatiotemporally controlled modulation of phagocytic signaling pathways.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"98 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701131","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":"Understanding the Electrocatalytic Trend of Sulfur Reduction Reaction and Design Rules of Advanced Electrocatalysts for Li-S Batteries.","authors":"Won-Gwang Lim,Seongbeen Kim,Miyeon Kim,Ara Cho,Minkyeong Ban,Cheol-Young Park,Donghyeok Son,Jeong Woo Han,Jinwoo Lee","doi":"10.1021/acsnano.5c05200","DOIUrl":"https://doi.org/10.1021/acsnano.5c05200","url":null,"abstract":"Despite the great potential of using electrocatalysts to improve the performance of lithium-sulfur (Li-S) batteries, a deficient understanding of the electrocatalytic trends in the sulfur reduction reaction with respect to the adsorption energy of sulfur active species and a lack of descriptors to estimate electrocatalytic activity limit the design of advanced electrocatalysts for Li-S batteries. Herein, we systematically explore the impact of sulfur species adsorption energy on the electrocatalytic activity in Li-S batteries by modulating the metal d-band structure of Pt3M (M = Cu, Fe, Ti, Co) alloy model systems. The Pt3Co catalyst, possessing a balanced d-band center, exhibited the highest redox kinetics and Li-S cell performance due to its lowest energy barrier for the rate-determining step in the sulfur reduction reaction. Furthermore, the adsorption energies of sulfur (S) and lithium (Li) single atoms can offer deeper insights into the electrocatalytic activity in Li-S electrochemistry, indicating their great potential as descriptors to develop advanced electrocatalysts. The volcano-type correlation of the d-band center and descriptor with the kinetics of the sulfur reduction reaction highlighted that moderate adsorption of Li and S on the catalyst surface with a balanced d-band center is the key to achieving optimal Li-S battery performance. This work emphasizes the importance of tailoring the surface properties and electronic structures of the electrocatalyst according to the intrinsic characteristics of electrocatalysts.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"33 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701166","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}
ACS NanoPub Date : 2025-07-24DOI: 10.1021/acsnano.5c09431
Sarah Z Khairunnisa,Olga Guselnikova,Yunqing Kang,Pavel S Postnikov,Rashid R Valiev,Jonathan P Hill,Nugraha Nugraha,Brian Yuliarto,Yusuke Yamauchi,Joel Henzie
{"title":"Hyperuniform Mesoporous Gold Films Coated with Halogen-Bonding Metal-Organic Frameworks for Selective Raman Sensing of Chlorinated Hydrocarbons.","authors":"Sarah Z Khairunnisa,Olga Guselnikova,Yunqing Kang,Pavel S Postnikov,Rashid R Valiev,Jonathan P Hill,Nugraha Nugraha,Brian Yuliarto,Yusuke Yamauchi,Joel Henzie","doi":"10.1021/acsnano.5c09431","DOIUrl":"https://doi.org/10.1021/acsnano.5c09431","url":null,"abstract":"The selective detection of chlorinated aromatic hydrocarbons (CAHs) in environmental samples is challenging due to matrix interference effects. We report a surface-enhanced Raman spectroscopy (SERS) sensor that combines mesoporous Au films with UiO-66-I metal-organic framework (MOF) coatings to achieve the selective detection of CAHs. We show that mesoporous Au films can be considered hyperuniform two-dimensional (2D) materials where long-range correlations and local disorder assist in electromagnetic hotspot formation for SERS. Infiltrating the mesoporous Au films with UiO-66-I serves dual functions critical to sensor performance: First, its iodine-functionalized linkers selectively recruit CAHs from complex matrices through halogen bonding (HaB), concentrating target molecules at SERS hotspots while excluding common interferents. Second, the high refractive index of the MOF enhances light coupling by limiting scattered light, concentrating optical energy on the adsorbed CAHs for SERS enhancement. At optimal MOF thickness, the sensor achieves a detection limit below 1 × 10-10 M for 1,4-dichlorobenzene and 4-chlorobiphenyl, surpassing environmental standards by several orders of magnitude. The sensor demonstrates excellent selectivity for CAHs over common interferents, including protein, polycyclic aromatic hydrocarbons, and complex environmental matrices. Furthermore, the sensor maintains performance through multiple adsorption-desorption cycles, enabling reuse. This approach combines reticular chemistry with self-assembled nanostructured metals to achieve both high sensitivity and selectivity in complex environmental samples.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"244 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693550","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":"Using the Electronic Grab-Transport Mechanism to Construct Metal-Organic Frameworks with Type I/II Dual Sonodynamic Therapy Reinforcement.","authors":"Xiang Jiang,Lina Sun,Yuewu Zhao,Zhiyong Lu,Xuan He,Ying Xiang,Xingzhu Liu,Jine Wang,Renjun Pei","doi":"10.1021/acsnano.5c05276","DOIUrl":"https://doi.org/10.1021/acsnano.5c05276","url":null,"abstract":"Sonodynamic therapy (SDT) has demonstrated promising potential in the treatment of tumors and has attracted widespread attention. The majority of sound-sensitive materials developed to date have been categorized as oxygen-dependent type II sonosensitizers (SSs), which are susceptible to tumor hypoxia and significantly limit their efficacy. In this study, highly active porphyrin-based metal-organic frameworks (Yb-TCPP PMOF) with type I/II SDT dual actions were constructed by regulating the electron transfer process between metal nodes and ligands, which can produce multiple reactive oxygen species (ROS) such as 1O2, O2•-, and •OH. After that, the energy level barrier of triplet SSs was reduced by in situ loading of Au nanoparticles with the electronic grab-transport (EGT) effect, and the ROS yield was increased by accelerating the electron transport. Intriguingly, the successful construction of Au/Yb-TCPP not only produced abundant oxygen vacancy defects but also reduced the band gap, which effectively facilitated the electron-hole separation of SSs and further improved the SDT efficiency by inhibiting its recombination process. Furthermore, we also found that these ultrasmall Au nanoparticles in the MOF structure can act as catalase and undergo cascade reactions with glucose oxidase and obtain a self-producing oxygen circulation system (Au/Yb-TCPP@GOx) by reducing glucose through the coordination of nanoenzyme and bioenzyme. This not only significantly alleviates the hypoxia state of tumors but also has a starvation effect on tumor cells. Finally, it was verified at the levels of tumor cells and mice that Au/Yb-TCPP@GOx can effectively inhibit tumors through the dual effects of enhanced type I and type II SDT, as well as the starvation effect. The composite materials constructed showed a multisynergistic enhancement effect, which has guiding significance for improving electron transport, alleviating tumor hypoxia, enhancing ROS yield, and constructing starvation treatment strategies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"25 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693595","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}