Zongliang Wan,Zheng Ji,Ruonan Tan,Suixin Zhang,Jingjing Gu,Cen-Feng Fu,Jin Ran
The poorly solvated nature of Li+ induces a strong interfacial affinity at the walls of the two-dimensional (2D) confined channels, a phenomenon referred to as the "chaotropic effect". This phenomenon severely hinders the transport of Li+ by creating substantial interfacial barriers, thereby compromising the Li+/Mg2+ separation efficiency. To tackle this challenge, we developed a strategy of grafting charged groups, such as sulfonates, onto the walls of graphene oxide (GO) channels. Theoretical simulations demonstrate that the Coulomb attraction between the negatively charged sulfonates and Li+ effectively repositions Li+ away from the channel walls toward the central region. This strategic redistribution of Li+ reduces the unfavorable Li+-wall interaction energy from -31.18 kJ/mol to -5.26 kJ/mol and suppresses the Li+'s hydration shell reconfiguration by approximately 49%. We experimentally engineered a sulfonated GO membrane that yields an almost 2-order-of-magnitude enhancement in Li+/Mg2+ selectivity and concurrently boosts Li+ flux by a factor of 5 compared with the pristine GO membrane, further firmly validating the feasibility of our strategy. This work establishes a conceptual framework for realizing highly efficient ion separation through 2D membranes.
{"title":"Weakening Chaotropic Effect of Li+ in Two-Dimensional Confined Channels via Coulomb Interactions for Efficient Li+/Mg2+ Separation.","authors":"Zongliang Wan,Zheng Ji,Ruonan Tan,Suixin Zhang,Jingjing Gu,Cen-Feng Fu,Jin Ran","doi":"10.1021/acsnano.5c21440","DOIUrl":"https://doi.org/10.1021/acsnano.5c21440","url":null,"abstract":"The poorly solvated nature of Li+ induces a strong interfacial affinity at the walls of the two-dimensional (2D) confined channels, a phenomenon referred to as the \"chaotropic effect\". This phenomenon severely hinders the transport of Li+ by creating substantial interfacial barriers, thereby compromising the Li+/Mg2+ separation efficiency. To tackle this challenge, we developed a strategy of grafting charged groups, such as sulfonates, onto the walls of graphene oxide (GO) channels. Theoretical simulations demonstrate that the Coulomb attraction between the negatively charged sulfonates and Li+ effectively repositions Li+ away from the channel walls toward the central region. This strategic redistribution of Li+ reduces the unfavorable Li+-wall interaction energy from -31.18 kJ/mol to -5.26 kJ/mol and suppresses the Li+'s hydration shell reconfiguration by approximately 49%. We experimentally engineered a sulfonated GO membrane that yields an almost 2-order-of-magnitude enhancement in Li+/Mg2+ selectivity and concurrently boosts Li+ flux by a factor of 5 compared with the pristine GO membrane, further firmly validating the feasibility of our strategy. This work establishes a conceptual framework for realizing highly efficient ion separation through 2D membranes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"310 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147518596","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}
Na4MnV(PO4)3 stands as a promising cathode material for sodium-ion batteries owing to its low cost and multiple redox potentials. However, challenges such as drastic local distortion, irreversible phase evolution, and transition metal dissolution in multielectron redox processes, coupled with intrinsic low electronic conductivity jointly trouble its practical deployment. Herein, the Ti4+ with a d0 arrangement is employed to customize the TM-O bonds to eliminate the structural distortion in Na4MnV(PO4)3. The coupling coordination effect of multiple transition metals activates the Mn4+/3+ redox while reinforcing structural stability in over two-electron redox processes, enabling the Na3.1(MnV)0.7Ti0.6(PO4)3 (MnVTi) cathode to realize a 2.4 e- reversible transfer and deliver a specific capacity of 138.4 mAh g-1. Experimental and theoretical calculations reveal that robust TM-O bonds with dynamic covalent chemistry, particularly the strong covalent Ti-O bonds, unlock ultrafast and durable cycling performance (78.4% capacity retention after 10,000 cycles at 20 C). Furthermore, the enhanced electronic conductivity and reaction kinetics contribute to the exceptional rate performance (74.2 mAh g-1 at 50 C), fast-charging capability (1.77 min to reach 80% SOC), and fabulous all-weather adaptability (-40 to 50 °C). This work establishes a universal design paradigm for high-performance Mn-based polyanion cathodes through d0-metal coupling mediated by dynamic covalent chemistry.
Na4MnV(PO4)3具有成本低、氧化还原电位高的优点，是一种很有前途的钠离子电池正极材料。然而，在多电子氧化还原过程中，剧烈的局部畸变、不可逆的相演变和过渡金属溶解等挑战，以及固有的低电子电导率共同阻碍了其实际应用。本文采用d0排列的Ti4+来定制TM-O键，以消除Na4MnV(PO4)3的结构畸变。多种过渡金属的偶联配位效应激活了Mn4+/3+氧化还原，同时增强了双电子氧化还原过程的结构稳定性，使Na3.1(MnV)0.7Ti0.6(PO4)3 （MnVTi）阴极实现了2.4 e-可逆转移，并提供了138.4 mAh g-1的比容量。实验和理论计算表明，具有动态共价化学的强大TM-O键，特别是强大的共价Ti-O键，解锁了超快和持久的循环性能（在20℃下循环10,000次后容量保持78.4%）。此外，增强的电子导电性和反应动力学有助于实现卓越的倍率性能（50℃时74.2 mAh g-1），快速充电能力（1.77分钟达到80% SOC）以及出色的全天候适应性（-40至50°C）。这项工作建立了一个通用的设计范式，通过动态共价化学介导的金属偶联来实现高性能锰基聚阴离子阴极。
{"title":"Dynamic Covalent Chemistry Eliminates Structural Distortion of Na4MnV(PO4)3: Unlocking Ultrafast and Durable Multielectron Redox in Sodium-Ion Batteries.","authors":"Miao Du,Ze-Lin Hao,Jia-Lin Yang,Xiao-Hua Zhang,Yan Liu,Xin-Yi Zhang,Xue-Jiao Nie,Dai-Huo Liu,Jin-Zhi Guo,Xing-Long Wu","doi":"10.1021/acsnano.6c00374","DOIUrl":"https://doi.org/10.1021/acsnano.6c00374","url":null,"abstract":"Na4MnV(PO4)3 stands as a promising cathode material for sodium-ion batteries owing to its low cost and multiple redox potentials. However, challenges such as drastic local distortion, irreversible phase evolution, and transition metal dissolution in multielectron redox processes, coupled with intrinsic low electronic conductivity jointly trouble its practical deployment. Herein, the Ti4+ with a d0 arrangement is employed to customize the TM-O bonds to eliminate the structural distortion in Na4MnV(PO4)3. The coupling coordination effect of multiple transition metals activates the Mn4+/3+ redox while reinforcing structural stability in over two-electron redox processes, enabling the Na3.1(MnV)0.7Ti0.6(PO4)3 (MnVTi) cathode to realize a 2.4 e- reversible transfer and deliver a specific capacity of 138.4 mAh g-1. Experimental and theoretical calculations reveal that robust TM-O bonds with dynamic covalent chemistry, particularly the strong covalent Ti-O bonds, unlock ultrafast and durable cycling performance (78.4% capacity retention after 10,000 cycles at 20 C). Furthermore, the enhanced electronic conductivity and reaction kinetics contribute to the exceptional rate performance (74.2 mAh g-1 at 50 C), fast-charging capability (1.77 min to reach 80% SOC), and fabulous all-weather adaptability (-40 to 50 °C). This work establishes a universal design paradigm for high-performance Mn-based polyanion cathodes through d0-metal coupling mediated by dynamic covalent chemistry.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"10 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147518593","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}
Chun Li,Vahid Shahed Gharahshiran,Jiarui Cui,Kaiyang Li,Yimin Zeng,Ying Zheng
Precise control over the coordination environment of single-atom catalysts remains a central challenge for steering multielectron electrocatalytic reactions. Here, we present oxygen-ligand programming─a chemical strategy that uses tailored surface carbonyl, hydroxyl, and carboxyl groups as programmable ligands to deterministically encode the coordination geometry and electronic configuration of atomic Cu anchored on carbon nanotubes. Atomic layer deposition on these ligand-defined interfaces generates chemically distinct Cu-O-C coordination motifs, whose electronic fingerprints are resolved by X-ray absorption spectroscopy. The programmed ligand fields selectively bias the stabilization of key intermediates: hydroxyl-derived motifs favor the O-bound *CONH species, carboxyl motifs overstabilize *NHx, while carbonyl-programmed motifs uniquely balance *CO and *NH2 adsorption, thereby unlocking efficient C-N coupling. This deterministic control over the reaction landscape yields a urea formation rate of 482 mg h-1 gcat-1 and a Faradaic efficiency of 61.2% at -0.6 V. Beyond urea synthesis, oxygen-ligand programming shows a broadly applicable conceptual framework for coordination-tailored single-atom catalysis and molecular pathway design in heterogeneous electrosynthesis.
{"title":"Programmable Oxygen-Ligand Fields Encode Atomic Cu Coordination for Pathway-Selective CO2-Nitrate Conversion to Urea.","authors":"Chun Li,Vahid Shahed Gharahshiran,Jiarui Cui,Kaiyang Li,Yimin Zeng,Ying Zheng","doi":"10.1021/acsnano.6c00620","DOIUrl":"https://doi.org/10.1021/acsnano.6c00620","url":null,"abstract":"Precise control over the coordination environment of single-atom catalysts remains a central challenge for steering multielectron electrocatalytic reactions. Here, we present oxygen-ligand programming─a chemical strategy that uses tailored surface carbonyl, hydroxyl, and carboxyl groups as programmable ligands to deterministically encode the coordination geometry and electronic configuration of atomic Cu anchored on carbon nanotubes. Atomic layer deposition on these ligand-defined interfaces generates chemically distinct Cu-O-C coordination motifs, whose electronic fingerprints are resolved by X-ray absorption spectroscopy. The programmed ligand fields selectively bias the stabilization of key intermediates: hydroxyl-derived motifs favor the O-bound *CONH species, carboxyl motifs overstabilize *NHx, while carbonyl-programmed motifs uniquely balance *CO and *NH2 adsorption, thereby unlocking efficient C-N coupling. This deterministic control over the reaction landscape yields a urea formation rate of 482 mg h-1 gcat-1 and a Faradaic efficiency of 61.2% at -0.6 V. Beyond urea synthesis, oxygen-ligand programming shows a broadly applicable conceptual framework for coordination-tailored single-atom catalysis and molecular pathway design in heterogeneous electrosynthesis.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"272 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147518597","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}
Rechargeable magnesium-sulfur (Mg-S) batteries are considered promising candidates for next-generation energy storage systems due to their intrinsic safety and natural abundance. However, their practical deployment is limited by the sluggish conversion of short-chain polysulfides, which contribute 75% of the theoretical capacity. Herein, cuprous tetrahydroxyquinone (Cu-THQ) is employed as an electrocatalyst anchored on a polypropylene interlayer to accelerate polysulfide conversion in Mg-S batteries. The restricted π-delocalization in the coordination framework and enhanced electron donation from oxygen atoms to Cu centers create the localized electron enrichment microenvironment and upshift the d-band center. This electronic modulation establishes an efficient charge-transfer pathway and strengthens Cu-S orbital hybridization, thereby facilitating the robust anchoring and accelerated reduction of MgS2 intermediates. Consequently, Mg-S batteries incorporating the Cu-THQ interlayer deliver a high reversible capacity of 470 mAh g-1 after 2000 cycles at 8.36 A g-1. Stable cycling performance is also maintained under -20 °C, demonstrating promising application potential. This work presents a π-conjugation-driven approach for accelerating polysulfide conversion and promotes the development of long-life Mg-S batteries.
可充电镁硫（Mg-S）电池由于其固有的安全性和天然丰度被认为是下一代储能系统的有希望的候选者。然而，它们的实际部署受到短链多硫化物转化缓慢的限制，短链多硫化物贡献了75%的理论容量。在本研究中，四羟基醌亚铜（Cu-THQ）作为电催化剂锚定在聚丙烯中间层上，以加速Mg-S电池中多硫化物的转化。配位框架中π离域的限制和氧原子向Cu中心的电子赋能的增强形成了局域电子富集微环境和d带中心的上移。这种电子调制建立了有效的电荷转移途径，加强了Cu-S轨道杂化，从而促进了MgS2中间体的稳健锚定和加速还原。因此，含有Cu-THQ中间层的Mg-S电池在8.36 a g-1下循环2000次后可提供高达470 mAh g-1的高可逆容量。在-20°C下也能保持稳定的循环性能，显示出良好的应用潜力。本文提出了一种π共轭驱动的加速多硫化物转化的方法，促进了长寿命Mg-S电池的发展。
{"title":"Constructing Charge Transfer Pathways via π-Conjugation Modulation for Long-Cycling Mg-S Batteries.","authors":"Xian Zhou,Tian Xu,Hongyu Zhang,Ming Sun,Zhihao Guo,Chaoqun Li,Mengshan Chen,Wenbin Wang,Miao Guo,Guanglin Xia,Xuebin Yu","doi":"10.1021/acsnano.6c00080","DOIUrl":"https://doi.org/10.1021/acsnano.6c00080","url":null,"abstract":"Rechargeable magnesium-sulfur (Mg-S) batteries are considered promising candidates for next-generation energy storage systems due to their intrinsic safety and natural abundance. However, their practical deployment is limited by the sluggish conversion of short-chain polysulfides, which contribute 75% of the theoretical capacity. Herein, cuprous tetrahydroxyquinone (Cu-THQ) is employed as an electrocatalyst anchored on a polypropylene interlayer to accelerate polysulfide conversion in Mg-S batteries. The restricted π-delocalization in the coordination framework and enhanced electron donation from oxygen atoms to Cu centers create the localized electron enrichment microenvironment and upshift the d-band center. This electronic modulation establishes an efficient charge-transfer pathway and strengthens Cu-S orbital hybridization, thereby facilitating the robust anchoring and accelerated reduction of MgS2 intermediates. Consequently, Mg-S batteries incorporating the Cu-THQ interlayer deliver a high reversible capacity of 470 mAh g-1 after 2000 cycles at 8.36 A g-1. Stable cycling performance is also maintained under -20 °C, demonstrating promising application potential. This work presents a π-conjugation-driven approach for accelerating polysulfide conversion and promotes the development of long-life Mg-S batteries.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"147 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147518598","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}
Hiroka Sugai, Shunsuke Tomita, Mariko Toyoda, Kota Watanuki, Mao Fukuyama, Takashi Kajitani, Kazushi Kinbara
Liquid–liquid phase separation (LLPS) plays a key role in cellular organization, enabling the formation of dynamic compartments that provide spatial and temporal control over biochemical processes. Although LLPS systems are typically fluidic, recent studies have revealed that specific molecular constituents can induce an internal structure. Here, we show that droplet formation between guanine quadruplexes (G4s) and polylysine peptides triggers G4-driven internal structural ordering. Using birefringence-retardation imaging, confocal fluorescence imaging, as well as X-ray diffraction and scattering techniques, we demonstrate that anisotropic subcompartments are gradually developed at specific points of their droplet–solution interfaces. The G4s possess intrinsic molecular rigidity due to their stacked G-quartet structures, and their interaction with the flexible polylysine peptides enables the formation of a hexagonal columnar phase (a = 3.64 nm; c = 0.86 nm; nine units per turn). This highly ordered subcompartment is enriched in low-fluidity G4s, while the peptides remain dynamically diffuse throughout the entire compartment. This supramolecular platform provides insights into the cooperative roles of structural order and molecular mobility in phase-separated systems, offering a foundation for the bottom-up design of synthetic condensates inspired by biomolecular organization.
液-液相分离（LLPS）在细胞组织中起着关键作用，使动态区室的形成能够提供对生化过程的空间和时间控制。虽然LLPS系统是典型的流体，但最近的研究表明，特定的分子成分可以诱导内部结构。在这里，我们发现鸟嘌呤四聚体（G4s）和聚赖氨酸肽之间的液滴形成触发g4驱动的内部结构排序。利用双折射-延迟成像、共聚焦荧光成像以及x射线衍射和散射技术，我们证明了各向异性子室在其液滴-溶液界面的特定点上逐渐发展。G4s由于其堆叠的g -四重奏结构而具有固有的分子刚性，并且它们与柔性聚赖氨酸肽的相互作用使其形成六方柱状相（a = 3.64 nm; c = 0.86 nm； 9个单位/转）。这个高度有序的亚室富含低流动性的G4s，而肽在整个室中保持动态扩散。这个超分子平台提供了对相分离体系中结构顺序和分子迁移率协同作用的见解，为受生物分子组织启发的自下而上的合成缩合物设计提供了基础。
{"title":"Emergence of Anisotropic Subcompartments via Coassembly of Hierarchically Ordered G-Quadruplexes and Fluid Polylysine in Droplet-Based Compartments","authors":"Hiroka Sugai, Shunsuke Tomita, Mariko Toyoda, Kota Watanuki, Mao Fukuyama, Takashi Kajitani, Kazushi Kinbara","doi":"10.1021/acsnano.5c21437","DOIUrl":"https://doi.org/10.1021/acsnano.5c21437","url":null,"abstract":"Liquid–liquid phase separation (LLPS) plays a key role in cellular organization, enabling the formation of dynamic compartments that provide spatial and temporal control over biochemical processes. Although LLPS systems are typically fluidic, recent studies have revealed that specific molecular constituents can induce an internal structure. Here, we show that droplet formation between guanine quadruplexes (G4s) and polylysine peptides triggers G4-driven internal structural ordering. Using birefringence-retardation imaging, confocal fluorescence imaging, as well as X-ray diffraction and scattering techniques, we demonstrate that anisotropic subcompartments are gradually developed at specific points of their droplet–solution interfaces. The G4s possess intrinsic molecular rigidity due to their stacked G-quartet structures, and their interaction with the flexible polylysine peptides enables the formation of a hexagonal columnar phase (<i>a</i> = 3.64 nm; <i>c</i> = 0.86 nm; nine units per turn). This highly ordered subcompartment is enriched in low-fluidity G4s, while the peptides remain dynamically diffuse throughout the entire compartment. This supramolecular platform provides insights into the cooperative roles of structural order and molecular mobility in phase-separated systems, offering a foundation for the bottom-up design of synthetic condensates inspired by biomolecular organization.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"9 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507475","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}
Detonation nanodiamonds containing silicon-vacancy (SiV) centers (SiV-DNDs) exhibit spectrally sharp optical transitions and are promising nanoscale emitters. After purification and oxidative postprocessing, SiV-DNDs are obtained with a mean particle diameter of ∼10 nm, a size scale at which single-color-center occupancy per particle may be expected. Yet, practical applications require selective enrichment from mixtures that also contain undoped nanodiamonds. Conventional separation methods lack sufficient selectivity, and resonant absorption-based optical sorting is fundamentally constrained by excited-state saturation, rendering it ineffective in the single-color-center regime. Building on our recent theoretical predictions that stimulated emission can generate a dissipative optical force beyond this limit, we demonstrate that the stimulated recoil force (SRF) provides a scalable mechanism for emission-line-selective manipulation of nanodiamonds in liquid. Using a glass capillary with counter-propagating pump beams and a manipulation beam resonant with SiV emission, we observe millimeter-scale downstream depletion and upstream enrichment of SiV-DNDs, while a spectrally distinct, off-resonant fluorescent nanodiamond population remains unchanged. The magnitude and spatial extent of the transport show that SRF overcomes Brownian diffusion and enables long-range, species-selective transport under realistic conditions. To identify the physical mechanism, we perform complementary glass-cell experiments under a well-defined focusing geometry and compare the observed enrichment with optical-force calculations based on density-matrix dynamics and Brownian-dynamics simulations. Qualitative agreement supports SRF as the dominant dissipative contribution responsible for the transport. These results demonstrate practical, emission-energy-selective optical sorting of fluorescent nanodiamonds and define design principles for extending this approach to capillaries, microfluidic systems, and other fluorescent nanomaterials.
{"title":"Selective Enrichment of Fluorescent Nanodiamonds by Stimulated Recoil Forces","authors":"Yoshiki Saito, Takao Horai, Yoshiki Umekawa, Ryosuke Shimono, Yoshihiro Tomoi, Takuya Matsuda, Yuto Makino, Yosuke Minowa, Hajime Ishihara, Masaaki Ashida","doi":"10.1021/acsnano.5c22759","DOIUrl":"https://doi.org/10.1021/acsnano.5c22759","url":null,"abstract":"Detonation nanodiamonds containing silicon-vacancy (SiV) centers (SiV-DNDs) exhibit spectrally sharp optical transitions and are promising nanoscale emitters. After purification and oxidative postprocessing, SiV-DNDs are obtained with a mean particle diameter of ∼10 nm, a size scale at which single-color-center occupancy per particle may be expected. Yet, practical applications require selective enrichment from mixtures that also contain undoped nanodiamonds. Conventional separation methods lack sufficient selectivity, and resonant absorption-based optical sorting is fundamentally constrained by excited-state saturation, rendering it ineffective in the single-color-center regime. Building on our recent theoretical predictions that stimulated emission can generate a dissipative optical force beyond this limit, we demonstrate that the stimulated recoil force (SRF) provides a scalable mechanism for emission-line-selective manipulation of nanodiamonds in liquid. Using a glass capillary with counter-propagating pump beams and a manipulation beam resonant with SiV emission, we observe millimeter-scale downstream depletion and upstream enrichment of SiV-DNDs, while a spectrally distinct, off-resonant fluorescent nanodiamond population remains unchanged. The magnitude and spatial extent of the transport show that SRF overcomes Brownian diffusion and enables long-range, species-selective transport under realistic conditions. To identify the physical mechanism, we perform complementary glass-cell experiments under a well-defined focusing geometry and compare the observed enrichment with optical-force calculations based on density-matrix dynamics and Brownian-dynamics simulations. Qualitative agreement supports SRF as the dominant dissipative contribution responsible for the transport. These results demonstrate practical, emission-energy-selective optical sorting of fluorescent nanodiamonds and define design principles for extending this approach to capillaries, microfluidic systems, and other fluorescent nanomaterials.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507476","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}
Wilanyi R Alvarez Reyes,Rima Jamous,Juliana Milagres,Rania El-Tanbouly,Raja Muthuramalingam Thangavelu,Vivian E Ferry,Washington da Silva,Christy L Haynes
Food insecurity is a prominent global issue. With a predicted global population of 9 billion by 2050, food production must double at a minimum to accommodate these growing numbers. One approach to combat food insecurity is targeting plant pathogens that affect crop quality and yield, resulting in an overall increase in edible food production. Plant pathogen management has previously utilized the RNA interference (RNAi) mechanism for remediation; however, its widespread use has technical limitations. In this study, silica nanoparticles (SiO2 NPs) were utilized as nanocarriers of therapeutic double-stranded ribonucleic acid (dsRNA) to enhance dsRNA delivery into plant cells, thereby activating the RNAi system and suppressing the occurrence of potato virus Y (PVY). This highly mutable pathogen causes several adverse effects in potato and other crop plants. Fast-dissolving silica (FDS) nanoparticles, mesoporous silica nanoparticles (MSNs), and ultraporous mesostructured silica nanoparticles (UMNs) with negative and positive surface charges were synthesized. After thorough characterization, nine distinct SiO2 NP formulations were loaded with dsRNA, with UMNs showing the best loading capacity. Due to the negatively charged nature of dsRNA, positively charged UMNs were favored and employed in further application experiments. Gel electrophoresis indicated that dsRNA loaded into/onto these UMNs was released over several days. Fifteen days after inoculation, greenhouse experiments with tobacco plants demonstrated that dsRNA-loaded UMNs effectively suppressed PVY. In a field study, dsRNA loaded into/onto UMNs showed a 0% disease incidence, an improvement compared to dsRNA or nanoparticle application alone. These findings reveal that UMNs are an efficient nanocarrier for delivering dsRNA against PVY, thereby increasing crop health and yield. A techno-economic analysis was performed to evaluate the economic viability of this nanomaterial for industrial commercialization.
{"title":"dsRNA-Loaded Silica Nanoparticles for the Management of Potato Virus Y in Potato Plants.","authors":"Wilanyi R Alvarez Reyes,Rima Jamous,Juliana Milagres,Rania El-Tanbouly,Raja Muthuramalingam Thangavelu,Vivian E Ferry,Washington da Silva,Christy L Haynes","doi":"10.1021/acsnano.5c19462","DOIUrl":"https://doi.org/10.1021/acsnano.5c19462","url":null,"abstract":"Food insecurity is a prominent global issue. With a predicted global population of 9 billion by 2050, food production must double at a minimum to accommodate these growing numbers. One approach to combat food insecurity is targeting plant pathogens that affect crop quality and yield, resulting in an overall increase in edible food production. Plant pathogen management has previously utilized the RNA interference (RNAi) mechanism for remediation; however, its widespread use has technical limitations. In this study, silica nanoparticles (SiO2 NPs) were utilized as nanocarriers of therapeutic double-stranded ribonucleic acid (dsRNA) to enhance dsRNA delivery into plant cells, thereby activating the RNAi system and suppressing the occurrence of potato virus Y (PVY). This highly mutable pathogen causes several adverse effects in potato and other crop plants. Fast-dissolving silica (FDS) nanoparticles, mesoporous silica nanoparticles (MSNs), and ultraporous mesostructured silica nanoparticles (UMNs) with negative and positive surface charges were synthesized. After thorough characterization, nine distinct SiO2 NP formulations were loaded with dsRNA, with UMNs showing the best loading capacity. Due to the negatively charged nature of dsRNA, positively charged UMNs were favored and employed in further application experiments. Gel electrophoresis indicated that dsRNA loaded into/onto these UMNs was released over several days. Fifteen days after inoculation, greenhouse experiments with tobacco plants demonstrated that dsRNA-loaded UMNs effectively suppressed PVY. In a field study, dsRNA loaded into/onto UMNs showed a 0% disease incidence, an improvement compared to dsRNA or nanoparticle application alone. These findings reveal that UMNs are an efficient nanocarrier for delivering dsRNA against PVY, thereby increasing crop health and yield. A techno-economic analysis was performed to evaluate the economic viability of this nanomaterial for industrial commercialization.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"7 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147518595","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}
Silicon exists in diverse chemical forms and, despite its low abundance in mammals, plays essential roles in skeletal and connective-tissue biology. Many marine organisms, particularly diatoms, have evolved sophisticated pathways for the controlled uptake, transport, and polymerization of silicic acid to generate mechanically robust, intricately patterned silica architectures. These natural systems challenge classical views of silicon as biologically inert and provide molecular blueprints for engineering silicon–biological interfaces. Advances in synthetic biology, mutagenesis, and materials science now enable rapid and programmable modulation of silicification beyond evolutionary time scales. This Perspective highlights recent progress across molecular, cellular, and tissue levels, outlining strategies, challenges, and opportunities for biosilicification as a platform to enhance biomaterial performance, preserve living systems, and integrate synthetic and biological matter.
{"title":"Biosilicification across Biological Hierarchies","authors":"Muyuyang Lin, Sishi Guo, Liang Zhou, Jiani Jiang, C. Jeffrey Brinker, Wei Zhu","doi":"10.1021/acsnano.5c22206","DOIUrl":"https://doi.org/10.1021/acsnano.5c22206","url":null,"abstract":"Silicon exists in diverse chemical forms and, despite its low abundance in mammals, plays essential roles in skeletal and connective-tissue biology. Many marine organisms, particularly diatoms, have evolved sophisticated pathways for the controlled uptake, transport, and polymerization of silicic acid to generate mechanically robust, intricately patterned silica architectures. These natural systems challenge classical views of silicon as biologically inert and provide molecular blueprints for engineering silicon–biological interfaces. Advances in synthetic biology, mutagenesis, and materials science now enable rapid and programmable modulation of silicification beyond evolutionary time scales. This Perspective highlights recent progress across molecular, cellular, and tissue levels, outlining strategies, challenges, and opportunities for biosilicification as a platform to enhance biomaterial performance, preserve living systems, and integrate synthetic and biological matter.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"58 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147519037","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}
Owen A. Vail,Shu-Wei Wang,Yasen Hou,Dinura Hettiarachchi,Jean-Félix Milette,Tim B. Eldred,Wenpei Gao,Wendy L. Sarney,Haile Ambaye,Jong Keum,Valeria Lauter,George J. de Coster,Matthew J. Gilbert,Don Heiman,Jagadeesh S. Moodera,Hang Chi
Magnetic topological insulators and their heterostructures provide significant opportunities to couple band topology with a nontrivial spin configuration for enhanced spintronic device performance, as well as designing magnetoelectric systems and functionalities. We find that Mn interdiffusion from MnTe when interfaced with (Bi,Sb)2Te3 stabilizes as self-organized Mn(Bi,Sb)2Te4 septuple lamellae among alternating (Bi,Sb)2Te3 quintuple layers, as observed using scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. We further demonstrate a valuable combination of magnetic and topological orders in these naturally formed Mn(Bi,Sb)2Te4–(Bi,Sb)2Te3 heterostructures, which are exchange-coupled with MnTe. Magnetotransport experiments and quantum magnetism simulations reveal that, above its own Néel temperature TN ∼ 20 K, Mn(Bi,Sb)2Te4 mediates the exchange field leading to an anomalous Hall effect at the (Bi,Sb)2Te3/MnTe interface, with an enhanced interfacial TN exceeding 200 K, approaching that of the bulk MnTe. This magnetic interface, in turn, allows a robust and deterministic spin–orbit torque switching without an external magnetic field at a low critical current density of 3 × 105 A cm–2. The antiferromagnetically coupled architecture of Mn(Bi,Sb)2Te4–(Bi,Sb)2Te3/MnTe, featuring magnetic and topological proximity effects across a chalcogenide backbone, is rich in fundamental interface physics and holds the potential for practical applications in spintronics.
{"title":"Proximity Magnetism in Mn(Bi,Sb)2Te4–(Bi,Sb)2Te3/MnTe Natural Heterostructures","authors":"Owen A. Vail,Shu-Wei Wang,Yasen Hou,Dinura Hettiarachchi,Jean-Félix Milette,Tim B. Eldred,Wenpei Gao,Wendy L. Sarney,Haile Ambaye,Jong Keum,Valeria Lauter,George J. de Coster,Matthew J. Gilbert,Don Heiman,Jagadeesh S. Moodera,Hang Chi","doi":"10.1021/acsnano.6c02294","DOIUrl":"https://doi.org/10.1021/acsnano.6c02294","url":null,"abstract":"Magnetic topological insulators and their heterostructures provide significant opportunities to couple band topology with a nontrivial spin configuration for enhanced spintronic device performance, as well as designing magnetoelectric systems and functionalities. We find that Mn interdiffusion from MnTe when interfaced with (Bi,Sb)2Te3 stabilizes as self-organized Mn(Bi,Sb)2Te4 septuple lamellae among alternating (Bi,Sb)2Te3 quintuple layers, as observed using scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. We further demonstrate a valuable combination of magnetic and topological orders in these naturally formed Mn(Bi,Sb)2Te4–(Bi,Sb)2Te3 heterostructures, which are exchange-coupled with MnTe. Magnetotransport experiments and quantum magnetism simulations reveal that, above its own Néel temperature TN ∼ 20 K, Mn(Bi,Sb)2Te4 mediates the exchange field leading to an anomalous Hall effect at the (Bi,Sb)2Te3/MnTe interface, with an enhanced interfacial TN exceeding 200 K, approaching that of the bulk MnTe. This magnetic interface, in turn, allows a robust and deterministic spin–orbit torque switching without an external magnetic field at a low critical current density of 3 × 105 A cm–2. The antiferromagnetically coupled architecture of Mn(Bi,Sb)2Te4–(Bi,Sb)2Te3/MnTe, featuring magnetic and topological proximity effects across a chalcogenide backbone, is rich in fundamental interface physics and holds the potential for practical applications in spintronics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506387","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}
Dohyun Lim,Hyeonseo Cheon,Seung Hwan Jeon,Min Woo Jeong,Yeon Soo Lee,Gui Won Hwang,Junwon Jang,Da Wan Kim,Jin Young Oh,Changhyun Pang
Skin-like wearable bioelectronics should exhibit stable adhesion, benign detachment, stretchability, and self-healability to meet the demands of future user-interactive electronic skin applications. Despite recent rapid advances in self-healable adhesive electronic materials, inherent flowability and fast chain dynamics still lead to inferior performance compared to nonself-healable systems. Herein, we present an architecturally stable, repositionable, and biocompatible reflow-controlled double-layered cephalopod-inspired adhesive electrode capable of autonomous self-healing. The reflow-resistant composite material consists of single-walled carbon nanotubes and supramolecular polymers that can control flowability and induce hierarchically self-assembled reinforced nanostructures, resulting in soft (Young’s modulus: ∼425 kPa) yet dimensionally stable systems under various conditions (underwater, pressure, and mild heat) over 7 days. The versatile bioelectronic adhesive interface programmed based on surface adaptability and energy distribution can induce robust adhesion in various (wet, rough, and dynamic) environments. Based on intimate adhesion with the skin, we demonstrate electrocardiogram/electromyogram signal acquisition and robot manipulation during dynamic motion under swollen, aged, and healed conditions.
{"title":"Conductive Reflow-Resistant Self-Healing Nanocomposite-Structured Adhesives for Reliable and Versatile Bioelectronic Interfaces","authors":"Dohyun Lim,Hyeonseo Cheon,Seung Hwan Jeon,Min Woo Jeong,Yeon Soo Lee,Gui Won Hwang,Junwon Jang,Da Wan Kim,Jin Young Oh,Changhyun Pang","doi":"10.1021/acsnano.5c18220","DOIUrl":"https://doi.org/10.1021/acsnano.5c18220","url":null,"abstract":"Skin-like wearable bioelectronics should exhibit stable adhesion, benign detachment, stretchability, and self-healability to meet the demands of future user-interactive electronic skin applications. Despite recent rapid advances in self-healable adhesive electronic materials, inherent flowability and fast chain dynamics still lead to inferior performance compared to nonself-healable systems. Herein, we present an architecturally stable, repositionable, and biocompatible reflow-controlled double-layered cephalopod-inspired adhesive electrode capable of autonomous self-healing. The reflow-resistant composite material consists of single-walled carbon nanotubes and supramolecular polymers that can control flowability and induce hierarchically self-assembled reinforced nanostructures, resulting in soft (Young’s modulus: ∼425 kPa) yet dimensionally stable systems under various conditions (underwater, pressure, and mild heat) over 7 days. The versatile bioelectronic adhesive interface programmed based on surface adaptability and energy distribution can induce robust adhesion in various (wet, rough, and dynamic) environments. Based on intimate adhesion with the skin, we demonstrate electrocardiogram/electromyogram signal acquisition and robot manipulation during dynamic motion under swollen, aged, and healed conditions.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"59 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506390","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：