ACS Nano最新文献

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MonitoringLiquid Concentration Changes in NanofluidicChannels Using Cross-Grating Wavefront Microscopy 利用交叉光栅波前显微镜监测纳米流体通道中液体浓度的变化
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c12559
Lova Wilske,Baptiste Marthy,Puvaneswari Teluchina-Appadu,Joachim Fritzsche,Guillaume Baffou,Christoph Langhammer
{"title":"Monitoring\u0000Liquid Concentration Changes in Nanofluidic\u0000Channels Using Cross-Grating Wavefront Microscopy","authors":"Lova Wilske,Baptiste Marthy,Puvaneswari Teluchina-Appadu,Joachim Fritzsche,Guillaume Baffou,Christoph Langhammer","doi":"10.1021/acsnano.6c12559","DOIUrl":"https://doi.org/10.1021/acsnano.6c12559","url":null,"abstract":"Abstract Optical microscopy that employs intensity measurements of scattered, transmitted, or emitted light is critical to study micro- and nanofluidic systems widely used in, e.g., biology, chemistry, and materials science. Since such fluidic systems often are transparent, simple bright-field microscopy observations are bound to yield low-contrast images. Fluorescence labeling or Raman imaging can be used to overcome this limitation and yield high contrast. However, these approaches are invasive or complex and slow and do not yield direct quantitative information about a liquid inside a micro- or nanofluidic structure. Quantitative phase microscopy techniques on the other hand are very efficient in enhancing the contrast of transparent samples, in a noninvasive manner. However, they have never been applied to nanofluidic systems. To fill this gap, we demonstrate how cross-grating wavefront microscopy enables the quantitative characterization of liquids in terms of concentration and refractive index, as well as solute diffusion, inside a single nanofluidic channel embedded in a SiO2 matrix in general and from diffraction-limited nanofluidic channel volume fractions as small as ∼45 aL. In a wider perspective, this study thus demonstrates the applicability of cross-grating wavefront microscopy to the characterization of processes taking place in volumes smaller than the diffraction limit of light, such as, e.g., nanofluidic systems, nanopores, or nanocavities.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"42 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209970","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}
引用次数: 0
FlexibleSingle-Walled Carbon Nanotube Film with UltrahighAbsolute Electromagnetic Shielding Performance 具有超高绝对电磁屏蔽性能的柔性单壁碳纳米管薄膜
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c13183
Zhi Liu,Zhong-Qiang Ni,Jia-Yang Zhang,Yu Meng,Zhao-Qing Gao,An-Ping Wu,Di Wang,Peng-Xiang Hou,Chang Liu
{"title":"Flexible\u0000Single-Walled Carbon Nanotube Film with Ultrahigh\u0000Absolute Electromagnetic Shielding Performance","authors":"Zhi Liu,Zhong-Qiang Ni,Jia-Yang Zhang,Yu Meng,Zhao-Qing Gao,An-Ping Wu,Di Wang,Peng-Xiang Hou,Chang Liu","doi":"10.1021/acsnano.6c13183","DOIUrl":"https://doi.org/10.1021/acsnano.6c13183","url":null,"abstract":"Abstract The rapid development of wearable electronic devices and fifth-generation (5G) communications have stimulated an urgent demand for flexible electromagnetic interference (EMI) shielding materials. Conventional metal-based EMI shielding materials typically fail to concurrently achieve good flexibility and effective EMI shielding performance. In this study, we prepared single-walled carbon nanotube (SWCNT) films comprising high-purity, high-crystallinity and high-aspect-ratio SWCNTs by floating catalyst chemical vapor deposition (FCCVD) followed by gas-phase purification. The obtained SWCNT film showed good flexibility, low density, and high electrical conductivity. A record-high absolute EMI shielding effectiveness (EMI SSE/t) of 5.42 × 105 dB·cm2/g and an exceptional normalized EMI shielding effectiveness (EMI SE/t) of 2.93 × 105 dB/cm, about twice as high as the highest reported EMI SSE/t value, were achieved for our SWCNT films. These results demonstrate that SWCNT films can be an ideal flexible EMI shielding material for use in next-generation wearable electronics and 5G communication systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209927","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}
引用次数: 0
In Vivo Blood Kineticsand Transcript Integrity ofThree mRNA–Lipid Nanoparticle Vaccines in Humans 三种mrna -脂质纳米颗粒疫苗在人体内的血液动力学和转录物完整性
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c09226
Stephen J. Kent,Shiyao Li,Thakshila H. Amarasena,Arnold Reynaldi,Michael G. Leeming,Jennifer A. Juno,Adam K. Wheatley,Georgia Deliyannis,Dale I. Godfrey,Terry Nolan,Colin W. Pouton,Miles P. Davenport,Yi Ju
{"title":"In Vivo Blood Kinetics\u0000and Transcript Integrity of\u0000Three mRNA–Lipid Nanoparticle Vaccines in Humans","authors":"Stephen J. Kent,Shiyao Li,Thakshila H. Amarasena,Arnold Reynaldi,Michael G. Leeming,Jennifer A. Juno,Adam K. Wheatley,Georgia Deliyannis,Dale I. Godfrey,Terry Nolan,Colin W. Pouton,Miles P. Davenport,Yi Ju","doi":"10.1021/acsnano.6c09226","DOIUrl":"https://doi.org/10.1021/acsnano.6c09226","url":null,"abstract":"Abstract mRNA–lipid nanoparticle (LNP) vaccines are detectable in human blood after vaccination, but platform-specific differences in systemic persistence and transcript integrity remain poorly defined. We analyzed serial blood samples from 73 participants receiving Moderna mRNA-1273 (three formulations), Pfizer/BioNTech BNT162b2, or an investigational receptor-binding domain (RBD) mRNA vaccine (three different doses). Using droplet digital polymerase chain reaction (ddPCR) assays, we quantified total and long-range linked (“intact”) vaccine mRNA, and we measured vaccine-specific ionizable lipids by liquid chromatography–mass spectrometry (LC–MS). Across platforms, mRNA decay was fastest for mRNA-1273, intermediate for BNT162b2, and slowest for the RBD vaccine, with ionizable lipid decay following the same rank order. Notably, intact spike mRNA declined 2-fold faster after mRNA-1273 than BNT162b2 vaccination. Kinetics modeling revealed platform-dependent coupling of mRNA and lipid kinetics: intact mRNA tracked closely with SM-102 for mRNA-1273, whereas ALC-0315 persisted longer than intact mRNA for BNT162b2. A ten-fragment linkage ddPCR panel spanning the spike transcript showed lower linkage toward 3′-proximal regions that mirrored the administered mRNA-1273 formulation. Together, these data provide a quantitative framework for benchmarking mRNA–LNP platform kinetics and transcript integrity in humans.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209966","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}
引用次数: 0
Symmetry-DirectedEngineering of Quantum Defects:Toward Monodispersed Organic Color Centers in Carbon Nanotubes 量子缺陷的对称定向工程:碳纳米管中单分散有机色心
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c07965
Mengyue Wang,Jacob Fortner,Benjamin Barnes,Daichi Kozawa,Chee Fai Fong,Jeffrey A. Fagan,Yuichiro K. Kato,YuHuang Wang
{"title":"Symmetry-Directed\u0000Engineering of Quantum Defects:\u0000Toward Monodispersed Organic Color Centers in Carbon Nanotubes","authors":"Mengyue Wang,Jacob Fortner,Benjamin Barnes,Daichi Kozawa,Chee Fai Fong,Jeffrey A. Fagan,Yuichiro K. Kato,YuHuang Wang","doi":"10.1021/acsnano.6c07965","DOIUrl":"https://doi.org/10.1021/acsnano.6c07965","url":null,"abstract":"Abstract Achieving spectrally uniform single-photon emission is crucial for scalable quantum photonics, yet conventional approaches often yield broad and unpredictable emission. Here, we report on the selective creation of organic color centers (OCCs) on high-symmetry zigzag (10,0) single-walled carbon nanotubes via a [2 + 2] cycloaddition reaction with 4-cyclopentene-1,3-dione. Density functional theory predicts two possible OCC binding configurations separated by >200 meV, favoring the selective formation of a single OCC geometry. Through chirality sorting, hyperspectral photoluminescence imaging, and multi-step spectral screening, we isolate functionalized (10,0) nanotubes and observe a substantially narrower distribution of OCC emission wavelengths than similarly functionalized chiral nanotubes. Time-resolved photoluminescence and photon correlation measurements further confirm single-photon emission at room temperature. These results demonstrate divalent OCCs on symmetric nanotubes as promising quantum emitters, offering a route toward scalable atomically defined light sources for integrated photonics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209925","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}
引用次数: 0
FluorescenceEncoding-Enabled Multiplexed DropletDigital Recombinase Polymerase Amplification-CRISPR/Cas12a Assay forRapid Screening of Lower Respiratory Tract Infection-Associated BacterialPathogens 荧光编码复用液滴数字重组酶聚合酶扩增- crispr /Cas12a快速筛选下呼吸道感染相关细菌病原体
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c13618
Yifan Wang,Enqi Huang,Ziyi Zhang,Xicong Zhu,Ting Zhang,Na Yang,Zhenhua Chen,Dongyang Cai,Dayu Liu
{"title":"Fluorescence\u0000Encoding-Enabled Multiplexed Droplet\u0000Digital Recombinase Polymerase Amplification-CRISPR/Cas12a Assay for\u0000Rapid Screening of Lower Respiratory Tract Infection-Associated Bacterial\u0000Pathogens","authors":"Yifan Wang,Enqi Huang,Ziyi Zhang,Xicong Zhu,Ting Zhang,Na Yang,Zhenhua Chen,Dongyang Cai,Dayu Liu","doi":"10.1021/acsnano.6c13618","DOIUrl":"https://doi.org/10.1021/acsnano.6c13618","url":null,"abstract":"Abstract Digital RPA-CRISPR/Cas12a assays enable accurate nucleic acid quantification; however, their multiplexing capacity is inherently limited by signal confounding arising from the promiscuous trans-cleavage activity of Cas12a effectors. To overcome this limitation, we developed a fluorescence encoding-enabled multiplexed droplet digital RPA-CRISPR/Cas12a (FLEMD-CRISPR) assay that integrates combinatorial fluorescence encoding, deterministic droplet pairing within a calabash-shaped microwell array, and a machine learning-assisted decoding pipeline. In FLEMD-CRISPR, small-volume fluorescence-encoded CRISPR/Cas12a droplets, each assigned a unique spectral signature corresponding to a specific crRNA, are one-to-one paired with large-volume RPA droplets. Following RPA amplification and droplet merging, Cas12a-mediated reporter cleavage occurs only in droplets containing target amplicons. The decoding pipeline then localizes droplets, classifies their colors to assign crRNA identities, and finally detects positive signals, enabling high-throughput, hands-off analysis of the entire droplet array. FLEMD-CRISPR enabled simultaneous quantification of nucleic acid targets from eight major lower respiratory tract infection-associated bacterial pathogens, showing strong linear correlation (R2 = 0.9987–0.9998) and consistent detection efficiency (slopes = 0.9849–1.0198) relative to single-plex digital PCR. The complete workflow, from sample preparation to final readout, can be completed within 2 h. Clinical validation using 30 bronchoalveolar lavage fluid samples showed that the bacterial detection outcomes of FLEMD-CRISPR were highly concordant with standard-of-care culture, achieving 100% (20/20) positive percent agreement and 99.1% (218/220) negative percent agreement. By enabling panel reconfiguration through simple modifications of the droplet encoding library, FLEMD-CRISPR provides a flexible platform for the development of highly multiplexed digital CRISPR assays.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"64 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209930","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}
引用次数: 0
Accelerated Screeningof Dimension-Controlled Cu3– y A y VS4– x Se x (A= K, Rb, Cs) via Soft Chemistry 软化学加速筛选尺寸控制Cu3 - y A y VS4 - x Se x (A= K, Rb, Cs
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c08880
Zhaohong Sun,Milo V. Carroll,Yizhen Chen,Zihang Sun,Ariana Nygren,Peter P. Russell,Romain Claes,Alexander G. Squires,Urvi Joshi,David O. Scanlon,Richard L. Brutchey
{"title":"Accelerated Screening\u0000of Dimension-Controlled Cu3–\u0000 y\u0000 A\u0000 y\u0000 VS4–\u0000 x\u0000 Se\u0000 x\u0000 (A\u0000= K, Rb, Cs) via Soft Chemistry","authors":"Zhaohong Sun,Milo V. Carroll,Yizhen Chen,Zihang Sun,Ariana Nygren,Peter P. Russell,Romain Claes,Alexander G. Squires,Urvi Joshi,David O. Scanlon,Richard L. Brutchey","doi":"10.1021/acsnano.6c08880","DOIUrl":"https://doi.org/10.1021/acsnano.6c08880","url":null,"abstract":"Abstract Dimension-driven design offers a powerful strategy for tuning the electronic structure of multinary chalcogenides, yet its application to solar absorbers remains limited. Previously explored systems lack candidates with optimal band gaps, while the time-consuming nature of solid-state synthesis impedes rapid synthesis and characterization of high-purity materials. Here, we report a colloidal soft-chemistry approach to systematically explore the Cu3–yAyVS4–xSex (A = K, Rb, Cs; y = 0, 1, 2; 0 ≤ x ≤ 3.5) compositional space, enabling simultaneous control over structural dimensionality (y), alkali-metal composition (A+), and chalcogen ratio (x) within a unified synthetic framework. By varying only precursor ratios, we access a broad family of phases spanning three-dimensional (3D), two-dimensional (2D), and one-dimensional (1D) [Cu–V–S] frameworks, as well as highly complex septenary solid solutions such as Cu(K, Rb, Cs)2VS2Se2. The resulting materials exhibit x-, y-, and A+-dependent optoelectronic properties, with band gaps tunable within the solar-relevant range of 1.40–1.67 eV, favorable band-edge alignment with CdS buffer layers, and intrinsic photocurrent responses. Theoretical calculations further elucidate the energy landscape and band structures of the understudied 1D series. Temperature- and time-resolved aliquot studies reveal pathway-dependent formation mechanisms, including direct nucleation of sulvanite Cu3VS4 and a two-step alkali-metal incorporation process governing the formation of alkali-metal-containing structures, providing key insights for related multinary chalcogenide systems. Overall, this work establishes a versatile platform for efficiently screening composition–structure–property relationships in complex chalcogenides for optoelectronic applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"24 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209932","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}
引用次数: 0
Low-Pb SubstitutionUnlocks Cd-Based Ruddlesden–PopperPerovskites for Bright Emission and Ambipolar Transport 低pb取代解锁基于cd的ruddlesden - popper钙钛矿的亮发射和双极输运
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c07579
Zisheng Tang,Zhe Pang,Damin Liu,Xiaoqian Wang,Jieheng Lv,Dafu Zhao,Manrui Liu,Chengqi Liu,Jiaqian Que,Kefeiyang Hu,Chong Peng,Xingbo Huang,Yingfei Liu,Dongyuan Zhao,Yong Liu
{"title":"Low-Pb Substitution\u0000Unlocks Cd-Based Ruddlesden–Popper\u0000Perovskites for Bright Emission and Ambipolar Transport","authors":"Zisheng Tang,Zhe Pang,Damin Liu,Xiaoqian Wang,Jieheng Lv,Dafu Zhao,Manrui Liu,Chengqi Liu,Jiaqian Que,Kefeiyang Hu,Chong Peng,Xingbo Huang,Yingfei Liu,Dongyuan Zhao,Yong Liu","doi":"10.1021/acsnano.6c07579","DOIUrl":"https://doi.org/10.1021/acsnano.6c07579","url":null,"abstract":"Abstract Two-dimensional (2D) Ruddlesden–Popper (RP) Cd-based perovskites have attracted increasing interest in optoelectronics owing to their environmental stability and tunable structural dimensionality. However, strong excited-state localization, abundant deep-level trap states, and inefficient carrier transport limit emission efficiency and device performance. Here, we report low-Pb-substituted 2D RP Cd-based perovskites, (PA)2CsCd2–xPbxCl7 (x = 0–0.4), and demonstrate that partial Pb2+ substitution provides an effective route to concurrently regulate luminescence and charge transport. At the optimal Pb2+ substitution level of x = 0.2, the photoluminescence quantum yield increases by approximately 7.6-fold, rising from 10.5% for the pristine sample to 80%. Steady-state and time-resolved photoluminescence analyses indicate a gradual redistribution from long-lived self-trapped exciton emission toward faster, higher-energy excitonic recombination. Field-effect transistors based on (PA)2CsCd1.8Pb0.2Cl7 exhibit pronounced ambipolar transport, with median hole and electron mobilities of 3.62 cm2 V–1 s–1 and 1.81 cm2 V–1 s–1, respectively, and a high on/off ratio of 8 × 107. Density functional theory calculations further reveal that Pb2+ substitution modulates the band-edge electronic states and suppresses the formation of deep-level defects. This work indicates that low-level Pb2+ substitution is an effective route for the concurrent optimization of luminescence and charge transport in Cd-based 2D perovskites, highlighting their potential for applications in high-performance transistors and light-emitting devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"39 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209926","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}
引用次数: 0
Seeing Inside aPlasmonic Nanogap: Few-Molecule Orientationand Preferential Adsorption 等离子体纳米间隙内部观察:少分子取向和优先吸附
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-15 DOI: 10.1021/acsnano.6c12575
Francesco Ciccarello,Nobuaki Oyamada,Thwahira Shirin Alampara,Konstantin Malchow,Christophe Galland
{"title":"Seeing Inside a\u0000Plasmonic Nanogap: Few-Molecule Orientation\u0000and Preferential Adsorption","authors":"Francesco Ciccarello,Nobuaki Oyamada,Thwahira Shirin Alampara,Konstantin Malchow,Christophe Galland","doi":"10.1021/acsnano.6c12575","DOIUrl":"https://doi.org/10.1021/acsnano.6c12575","url":null,"abstract":"Abstract Molecule–surface interactions are central to many research and technological areas, spanning from heterogeneous catalysis and polymer science to electrochemistry. Of particular relevance are metallic nanogaps used in molecular electronics and near-field spectroscopy. Due to the buried nature of these double interfaces, few methods exist to monitor side-specific interactions and relative molecular orientation inside the gap. In this work, we employ plasmon-enhanced nonlinear vibrational spectroscopy as an efficient tool to investigate surface molecular adsorption within metallic nanojunctions. By exploiting simultaneous vibrational sum- and difference-frequency generation in dual-resonant nanocavities, we resolve molecular orientation and preferential binding to one of the two gold surfaces, with few-molecule sensitivity. We also notice that the nonresonant (electronic) second-order nonlinear response is not an intrinsic property of the metal surface, but is instead governed by the molecule–surface interaction. Our findings provide a powerful analytical tool, easily implementable as an add-on to Raman spectroscopy, thanks to commercially available mid-infrared quantum cascade lasers.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"42 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209967","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}
引用次数: 0
Activity-Stability Balance Enabled by Orbital Splitting Energy in Ruthenium-Based Oxide Catalysts. 钌基氧化物催化剂的轨道分裂能激活活性-稳定性平衡。
IF 17.3 1区 材料科学
ACS Nano Pub Date : 2026-10-14 DOI: 10.1021/acsnano.6c16492
Qingyi Liu, Lifeng Hang, Jinwu Liu, Da-Qian Cai, Zhehan Yi, Tao Zhang, Ting Yu, Hong Jin Fan
{"title":"Activity-Stability Balance Enabled by Orbital Splitting Energy in Ruthenium-Based Oxide Catalysts.","authors":"Qingyi Liu, Lifeng Hang, Jinwu Liu, Da-Qian Cai, Zhehan Yi, Tao Zhang, Ting Yu, Hong Jin Fan","doi":"10.1021/acsnano.6c16492","DOIUrl":"https://doi.org/10.1021/acsnano.6c16492","url":null,"abstract":"<p><p>Ruthenium oxides have been the model catalyst for the acidic oxygen evolution reaction. It has been a challenge to achieve both stability and activity and establish a comprehensive descriptor for Ru-based catalysts. Herein, guided by the ligand field theory, we introduce the Ru orbital splitting energy (ΔRu) as a quantitative parameter to describe the interaction between Ru 4d and O 2p orbitals to govern the overall catalytic performance. A series of two-dimensional (2D) multielement metal oxides are synthesized via a self-assembly method to modulate ΔRu. The optimized RuCoFeNiO catalyst for water oxidation delivers a current density of 10 mA cm-2 at a low overpotential of 180 mV and shows high activity for more than 2500 h at 1 A cm-2 in acidic condition. In situ measurements and theoretical analysis reveal that the surface hydrogen-bond network balances the amount of surficial two-hydrogen-bonded water and free water, boosting the proton-transfer process. Moreover, the optimized ΔRu (2.405 eV) modifies the adsorption of *OOH on Ru sites, switching the dominant reaction pathway from the lattice oxygen mediated mechanism to absorbate evolution mechanism. This work highlights the pivotal role of ΔRu in tailoring both stability and activity and may offer insights into high-entropy 2D Ru-based oxides as high-performance oxygen evolution electrocatalysts.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":17.3,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149190231","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}
引用次数: 0
Breaking the High-VoltageLimit of Na2CO3 Presodiation: An InterfacialEngineering Approach to Ampere-HourSodium-Ion Devices 突破Na2CO3沉淀的高压限制:安培-小时钠离子器件的界面工程方法
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2026-10-14 DOI: 10.1021/acsnano.6c11812
Luoming Zhang,Biao Zhong,Xinyu Zhang,Yuming Liu,Junpu Zhang,Bo Xiong,Shengrui Gao,Dongxiao Li,Jie Li,Lei Sun,Wentao Deng,Hongshuai Hou,Xiaobo Ji,Guoqiang Zou
{"title":"Breaking the High-Voltage\u0000Limit of Na2CO3 Presodiation: An Interfacial\u0000Engineering Approach to Ampere-Hour\u0000Sodium-Ion Devices","authors":"Luoming Zhang,Biao Zhong,Xinyu Zhang,Yuming Liu,Junpu Zhang,Bo Xiong,Shengrui Gao,Dongxiao Li,Jie Li,Lei Sun,Wentao Deng,Hongshuai Hou,Xiaobo Ji,Guoqiang Zou","doi":"10.1021/acsnano.6c11812","DOIUrl":"https://doi.org/10.1021/acsnano.6c11812","url":null,"abstract":"Abstract Na2CO3 is a promising sacrificial presodiation agent owing to its high capacity, excellent air stability, and low cost. However, its practical application is severely hampered by a high decomposition overpotential (&amp;gt;4.3 V vs Na/Na+), inducing detrimental electrolyte oxidation and cell degradation. To break this high-voltage limit, we propose an in situ interfacial dual-modification strategy, synergistically introducing interfacial oxygen vacancies and triggering electronic reconstruction, which thermodynamically lowers the reaction Gibbs free energy and kinetically diminishes the activation barriers, resulting in a dramatically reduced decomposition potential by 350 mV. Operando three-electrode diagnostics within a full sodium-ion capacitor reveal that this interface engineering not only facilitates efficient Na+ release (496.9 mAh g–1) at lower potential but also reduces the actual working potential of cathode, thereby fundamentally avoiding high-voltage parasitic reactions, according well with the DEMS and TOF-SIMS results. Consequently, the full cell achieves a considerable 117.4% enhancement in energy density. Most importantly, this strategy demonstrates compelling practicality in ampere-hour-level devices, delivering a substantial 22.4% boost in energy density with only 3 wt % additive in 1.5 Ah pouch cells. This work bridges microscopic interfacial chemistry and macroscopic device performance, providing a scalable and efficient blueprint for low-potential presodiation toward high-energy-density sodium-ion devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209975","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}
引用次数: 0
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