ACS Nano最新文献

{"title":"Correlating Photo-Induced Changes in Surface Charge and Electronic Conductivity in Oxide Nanoparticles with In Situ Electron Microscopy.","authors":"Piyush Haluai,Martha R McCartney,Yifan Wang,Peter A Crozier","doi":"10.1021/acsnano.4c13539","DOIUrl":"https://doi.org/10.1021/acsnano.4c13539","url":null,"abstract":"Photon induced changes in charge distributions and conductivities of oxide nanoparticles (rhodium doped strontium titanate) have been determined using in situ electron holography. The holography-based approach relies on the application of two distinct stimuli to the material of interest: electrons and photons. The high energy electron beam stimulates the formation of a layer of positive surface charge due to secondary electron emission. Light illumination reduces this charge due to enhanced electronic conductivity arising from photoelectron excitation. For moderate photon and electron illumination rates, there is a simple linear relationship between the steady state surface charge and the sample conductivity. For rhodium doped strontium titanate, we observe a factor of 3 increase in the conductivity for the illumination conditions employed here. The approach is general and can be employed to measure photoinduced changes in other semiconducting systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103596","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":"Oxide Heterostructure Engineering Drives Stable Lattice Oxygen Evolution for Highly Efficient and Robust Water Electrolysis.","authors":"Chenghao Jia,Yan Chen,Chenyu Zhou,Xuepeng Xiang,Xin Long,Bin Zhao,Nian Zhang,Shijun Zhao,Liyuan Chai,Xueming Liu,Zhang Lin","doi":"10.1021/acsnano.5c03084","DOIUrl":"https://doi.org/10.1021/acsnano.5c03084","url":null,"abstract":"Achieving a highly active and stable oxygen evolution reaction (OER) is critical for the implementation of water electrolysis in green hydrogen production but remains challenging. Steering the OER pathway from an adsorbate evolution mechanism (AEM), where a metal site serves as the active site, to the lattice oxygen mechanism (LOM) has been found to enhance OER activity; however, it suffers from low stability. In this work, we propose to construct CuOx/Co3O4 heterointerface, which enables the realization of a stable LOM pathway. The lattice oxygen characteristics are modulated near the heterointerface, resulting in a shift in the reaction pathway from AEM to LOM. In situ X-ray Absorption Fine Structure results further reveal that the valence state of cobalt is stabilized during the OER process, which alleviates corrosion of cobalt and maintains LOM stability. Consequently, the obtained CuOx/Co3O4 exhibits outstanding activity and stability for overall water electrolysis in freshwater, natural seawater, and high-salt wastewater, with a low overpotential of 308 mV at 100 mA cm-2 and stable overall water electrolysis at 500 mA cm-2 for 100 h. Our work demonstrates interface engineering as an effective strategy to activate and stabilize lattice oxygen, advancing the design of high-performance electrocatalysts for energy and environmental applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"127 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103669","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-Protein Determinations by Magnetofluorescent Qubit Imaging with Artificial-Intelligence Augmentation at the Point-Of-Care.","authors":"Yaqi Huang,Wei Liu,Tiantian Man,Jinwei Du,Xianli Gong,Fujin Lv,Wenhao Shan,Lu Ding,Ying Wan,Shengyuan Deng","doi":"10.1021/acsnano.5c04340","DOIUrl":"https://doi.org/10.1021/acsnano.5c04340","url":null,"abstract":"Conventional point-of-care testing (POCT) has limitations in sensitivity with high risks of missed detection or false positive, which restrains its applications for routine outpatient care analysis and early clinical diagnosis. By merits of the cutting-edge quantum precision metrology, this study devised a mini quantum sensor via magnetofluorescent qubit tagging and tunning on core-shelled fluorescent nanodiamond FND@SiO2. Comprehensive characterizations confirmed the formation of FND biolabels, while spectroscopies secured no degradation in spin-state transition after surface modification. A methodical parametrization was deliberated and decided, accomplishing a wide-field modulation depth ≥15% in ∼ zero field, which laid foundation for supersensitive sensing at single-FND resolution. Using viral nucleocapsid protein as a model marker, an ultralow limit of detection (LOD) was obtained by lock-in analysis, outperforming conventional colorimetry and immunofluorescence by > 2000 fold. Multianalyte and affinity assays were also enabled on this platform. Further by resort to artificial-intelligence (AI) augmentation in the Unet-ConvLSTM-Attention architecture, authentic qubit dots were identified by pixelwise survey through pristine qubit queues. Such processing not just improved pronouncedly the probing precision but also achieved deterministic detections down to a single protein in human saliva with an ultimate LOD as much as 7800-times lower than that of colloidal Au approach, which competed with the RT-qPCR threshold and the certified critical value of SIMOA, the gold standard. Hence, by AI-aided digitization on optic qubits, this REASSURED-compliant contraption may promise a next-generation POCT solution with unparalleled sensitivity, speed, and cost-effectiveness, which in whole confers a conclusive proof of the prowess of the burgeoning quantum metrics in biosensing.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"32 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087576","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":"Enhancing Rechargeable Zinc-Air Batteries with Atomically Dispersed Zinc Iron Cobalt Planar Sites on Porous Nitrogen-Doped Carbon.","authors":"Rui Wu,Jiayu Zuo,Chuang Fu,Zhaozhao Zhu,Lei Zhao,Junjie Wang,Qiyu Li,Qian Xue,Zhao Li,Xiaobin Niu,Xueqiang Qi,Na Yang,Jun Song Chen","doi":"10.1021/acsnano.5c05961","DOIUrl":"https://doi.org/10.1021/acsnano.5c05961","url":null,"abstract":"Rechargeable zinc-air batteries (ZABs) face significant challenges in achieving both high power density and long-term stability, primarily due to limitations in catalytic materials for oxygen electrodes. Here, we present a trimetal planar heterogeneous metal catalyst featuring atomically dispersed ZnN4, FeN4, and CoN4 sites supported on a porous nitrogen-doped carbon substrate (ZnFeCo-NC) through a templating approach. By fine-tuning the content of each metal, the optimized ZnFeCo-NC-based ZAB achieves a high peak power density of 244 mW cm-2 and maintains durable performance for 500 h at 10 mA cm-2. Ab initio molecular dynamics simulations reveal that the ZnFeCo-NC catalyst configuration remains stable at 300 K during the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) process. Further theoretical calculations demonstrate that the introduction of adsorbed OH groups effectively tunes the electronic structure redistribution of metal active sites, particularly improving the catalytic performance at the Fe site for ORR and the Co site for the OER. These findings provide insights into the rational design of high-performance electrocatalysts in energy storage technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"13 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087579","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":"Machine Learning-Based Reward-Driven Tuning of Scanning Probe Microscopy: Toward Fully Automated Microscopy","authors":"Yu Liu, Roger Proksch, Jason Bemis, Utkarsh Pratiush, Astita Dubey, Mahshid Ahmadi, Reece Emery, Philip D. Rack, Yu-Chen Liu, Jan-Chi Yang, Sergei V. Kalinin","doi":"10.1021/acsnano.4c18760","DOIUrl":"https://doi.org/10.1021/acsnano.4c18760","url":null,"abstract":"Since the dawn of scanning probe microscopy (SPM), tapping or intermittent contact mode has been one of the most widely used imaging modes. Manual optimization of tapping mode not only takes a lot of instrument and operator time but also often leads to frequent probe and sample damage, poor image quality, and reproducibility issues for new types of samples or inexperienced users. Despite wide use, optimization of tapping mode imaging is an extremely difficult problem, being ill-suited to both classical control methods and machine learning techniques. Here, we describe a reward-driven workflow to automate the optimization of the SPM in tapping mode. The reward function is defined based on multiple channels with physical and empirical knowledge of good scans encoded, representing a sample-agnostic measure of image quality and imitating the decision-making logic employed by human operators. The workflow determines scanning parameters that produce consistent, high-quality images in attractive modes across various probes and samples. These results demonstrate improved efficiency and reliability in tapping mode SPM operation.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"18 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088109","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":"Intrinsic Exciton Transport and Recombination in Single-Crystal Lead Bromide Perovskite","authors":"Zhixuan Bi, Yunfei Bai, Ying Shi, Tao Sun, Heng Wu, Haochen Zhang, Yuhang Cui, Danlei Zhu, Yubin Wang, Miao-Ling Lin, Yaxian Wang, Dongxin Ma, Ping-Heng Tan, Sheng Meng, Qihua Xiong, Luyi Yang","doi":"10.1021/acsnano.5c03274","DOIUrl":"https://doi.org/10.1021/acsnano.5c03274","url":null,"abstract":"Photogenerated carrier transport and recombination in metal halide perovskites are critical to device performance. Despite considerable efforts, sample quality issues and measurement techniques have limited the access to their intrinsic physics. Here, by utilizing high-purity CsPbBr₃ single crystals and contact-free transient grating spectroscopy, we directly monitor exciton diffusive transport from 26 to 300 K. As the temperature (<i>T</i>) increases, the carrier mobility (μ) decreases rapidly below 100 K wtih a μ ∼ <i>T</i>^–3.0 scaling, and then follows a more gradual μ ∼ <i>T</i>^–1.7 trend at higher temperatures. First-principles calculations perfectly reproduce this experimental trend and reveal that optical phonon scattering governs carrier mobility shifts over the entire temperature range, with a single longitudinal optical mode dominating room-temperature transport. Time-resolved photoluminescence further identifies a substantial increase in exciton radiative lifetime with temperature, attributed to increased exciton population in momentum-dark states caused by phonon scattering. Our findings unambiguously resolve previous theory-experiment discrepancies, providing benchmarks for future optoelectronic design.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"10 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088110","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":"Cathodoluminescence Saturation Imaging to Visualize Emitter-Resonator Coupling.","authors":"Hikaru Saito,Yuuichiro Kimura,Kentaro Matsuzaki,Yoshikazu Adachi,Sotatsu Yanagimoto,Kosuke Watanabe,Miki Inada,Takumi Sannomiya","doi":"10.1021/acsnano.4c15144","DOIUrl":"https://doi.org/10.1021/acsnano.4c15144","url":null,"abstract":"Nanoscopic characterization of light-emitting materials is essential to realize nano-optical devices, which requires nanoscopic spatial resolution far beyond the diffraction limit of light. Cathodoluminescence (CL) is a powerful means to achieve such nano-optical characterization by combining with electron microscopy. However, discrimination between coherent and incoherent CL emissions, when a phosphor material is combined with a resonator, is not trivial. To solve this general problem in such coupled emitter-resonator systems, we take advantage of optical saturation in incoherent CL in the phosphor and propose a method to extract the incoherent component to distinguish the coherent components purely from the resonator. We demonstrate this CL saturation imaging approach using an integrated system of Zn2SiO4 phosphors and a plasmonic resonator array and visualize the resonator-modified luminescence at the nanoscale, which evidence the near-field coupling between the phosphors and the plasmonic resonators.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"22 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087583","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":"Breaking the Activity and Stability Trade-Off of Platinum-Free Catalysts for the Oxygen Reduction Reaction in Hydrogen Fuel Cells.","authors":"Shiyang Liu, Quentin Meyer, Dong Xu, Yi Cheng, Luigi Osmieri, Xin-Hao Li, Chuan Zhao","doi":"10.1021/acsnano.5c03610","DOIUrl":"https://doi.org/10.1021/acsnano.5c03610","url":null,"abstract":"<p><p>Hydrogen fuel cells, which use hydrogen as fuel to generate electricity, hold great promises as future energy conversion devices for heavy-duty transport, due to their zero CO₂ emissions, high energy conversion efficiency, and high power density. However, the adoption of hydrogen fuel cells has been slow due to their reliance on large amounts of costly and scarce platinum (Pt) for the oxygen reduction reaction. The replacement of Pt with Earth-abundant transition metals such as Fe, Co, Mn, and Sn with oxygen reduction reaction affinity has thus been a holy grail of electrocatalysis research. Pt-free catalysts must combine both high power density and high stability in hydrogen fuel cells to be considered viable alternatives to Pt. Despite promising progress on both fronts, a trade-off has emerged: Pt-free catalysts either achieve high power densities (≥1.5 W cm^-2) but suffer from low stabilities (≥70% loss after 25 h) or more recently demonstrate improved stability (≤25% loss after 150 h), while delivering considerably lower power densities (<1 W cm^-2) in hydrogen fuel cells. Herein, we summarize the recent progress in the synthesis of high power density M-N-C catalysts for hydrogen fuel cells and highlight the critical importance of uncovering the underlying mechanisms using <i>operando</i> methods. We then discuss the primary causes of catalyst degradation in hydrogen fuel cells and the most promising strategies to enhance the stability of the M-N-C catalysts. Finally, a roadmap is proposed to overcome the activity stability trade-off for Pt-free catalysts in hydrogen fuel cells.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144100962","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":"Enantiospecificity in Organic Photoelectrochemical Transistors Enabled by Chirality-Induced Spin Selectivity Effects.","authors":"Jian-Hong Zhu, Xinzhe Yang, Yulin Zheng, Shujia Wang, Zhen-Kun He, Zhida Gao, Yan-Yan Song","doi":"10.1021/acsnano.5c06982","DOIUrl":"https://doi.org/10.1021/acsnano.5c06982","url":null,"abstract":"<p><p>Chirality, as an intrinsic feature of the living world, is associated with many significant biological processes. Although the chiral-induced spin selectivity (CISS) effects have been recognized and applied to provide spin control over chemical reactions, their implementation in the organic electrochemical transistor (OECT) remains a largely unexplored area. Herein, the OECT technology is combined with a photovoltaic gate electrode and the CISS effect, establishing a chiral organic photoelectrochemical transistor (OPECT) for enantiomer identification. The chiral Sn(II)-based metal-organic framework (SnMOF)/SnO₂ hybrid, serving as a spin filter to induce CISS properties, is coated on a TiO₂ nanotube array-based photosensitive gate. Using cystine enantiomers as proof-of-principle, a target recognition-induced electron donor (l-/d-cysteine) generation was further proposed. The CISS effect enables a more efficient transfer of spin-polarized electrons between the L-target and L-gate (or between the D-target and D-gate), inducing a greater channel current (<i>I</i>_D) variation. The comprehensive analysis of the <i>I</i>_D responses in the two chiral OPECT sensors further enables accurate and reliable determination of the concentration and composition of enantiomers in unknown mixtures. This study provides a straightforward methodology to apply the CISS effect for determining chiral targets in complex samples.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144100964","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":"Liquid Metal Amplified Charge Separation in Photocatalytic Micro/Nanomotors for Antibacterial Therapy.","authors":"Zichang Guo,Dongdong Jin,Haohui Li,Xinyu Zhu,Tianqi Zheng,Zirong Xu,Yi Chen,Xiaojia Liu,Yinuo Song,Dai Wang,Xiaohui Yan,Xing Ma","doi":"10.1021/acsnano.5c03785","DOIUrl":"https://doi.org/10.1021/acsnano.5c03785","url":null,"abstract":"Photocatalytic micro/nanomotors (MNMs) driven by electrophoresis have attracted considerable attention by virtue of their active mobility and versatile functionality. However, the rapid recombination of photogenerated electron-hole pairs on light illumination severely compromises the involvement of charge species in the catalytic redox reactions of fuels, thus hindering both the propulsion and the application performance of photocatalytic MNMs. Herein, we report a facile strategy to amplify charge separation by incorporating liquid metal (LM) into the construction of photocatalytic MNMs, thereby strengthening the electrophoretic propulsion of MNMs and promoting the generation of reactive oxygen species (ROS) for antibacterial application. The MNMs are constructed with a gallium (Ga) LM core, coated with abundant graphite-phase carbon nitride (g-C3N4) nanosheets and half covered by a thin platinum layer. These MNMs exhibit self-propulsion in hydrogen peroxide (H2O2) solution, with their motion dynamics further enhanced by light irradiation. Theoretical calculations and simulations reveal that the composition between Ga and g-C3N4 forms an ohmic junction in the electronic energy band structure, which effectively improves the charge separation efficiency of electron-hole pairs. These results align well with the experimental electrochemical tests and consequently intensify the catalytic redox reactions of H2O2, as well as accelerate the charge migration across MNMs, contributing to the enhancement of their propulsion performance. Simultaneously, the amplified separation of electrons facilitates increased ROS generation, empowering the MNMs with motion-enhanced antibacterial activity against Escherichia coli. Finally, an in vivo wound healing experiment is conducted, verifying the superior antibacterial therapeutic performance of photocatalytic MNMs. This work not only provides insights into the role of charge species in phoretic motion of MNMs but also gives inspiration for developing photocatalytic MNMs with advanced biomedical applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"12 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097684","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}