Pub Date : 2025-12-04DOI: 10.1021/acs.nanolett.5c04791
Sultan Almunif, Simseok A. Yuk, El Hadji Arona Mbaye, Swagat Sharma, Michael D. Purdy, Sandeep Kumar, Natalie R. Klug, Evan A. Scott
Bicontinuous nanospheres (BCNs) are self-assembled nanostructures with interconnected aqueous channels that enable the coloading of hydrophilic and hydrophobic cargo; however, their size has been difficult to control. Here, we present a scalable approach to tune the size distribution of poly(ethylene glycol)-b-poly(propylene sulfide) BCNs using a multi-inlet vortex mixer. Higher mixing times and polymer concentrations produced larger BCNs, while shorter mixing times and lower concentrations yielded spherical micelles. Small-angle X-ray scattering and cryogenic transmission electron microscopy confirmed the BCN bicontinuous morphology, which persisted at smaller sizes. The porous BCN structure resulted in increased surface roughness compared to polymersomes (PSs). In vitro, BCNs and PSs of comparable sizes recruited distinct protein coronas early, but their profiles showed convergence by 24 h. In vivo, organ biodistribution was determined primarily by the nanocarrier size rather than the morphology. These findings establish a robust approach to BCN fabrication while revealing dynamic biological interactions that inform nanocarrier design.
{"title":"Engineering the Size of Bicontinuous Nanospheres via Multi-Inlet Vortex Mixing","authors":"Sultan Almunif, Simseok A. Yuk, El Hadji Arona Mbaye, Swagat Sharma, Michael D. Purdy, Sandeep Kumar, Natalie R. Klug, Evan A. Scott","doi":"10.1021/acs.nanolett.5c04791","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04791","url":null,"abstract":"Bicontinuous nanospheres (BCNs) are self-assembled nanostructures with interconnected aqueous channels that enable the coloading of hydrophilic and hydrophobic cargo; however, their size has been difficult to control. Here, we present a scalable approach to tune the size distribution of poly(ethylene glycol)-<i>b</i>-poly(propylene sulfide) BCNs using a multi-inlet vortex mixer. Higher mixing times and polymer concentrations produced larger BCNs, while shorter mixing times and lower concentrations yielded spherical micelles. Small-angle X-ray scattering and cryogenic transmission electron microscopy confirmed the BCN bicontinuous morphology, which persisted at smaller sizes. The porous BCN structure resulted in increased surface roughness compared to polymersomes (PSs). <i>In vitro</i>, BCNs and PSs of comparable sizes recruited distinct protein coronas early, but their profiles showed convergence by 24 h. <i>In vivo</i>, organ biodistribution was determined primarily by the nanocarrier size rather than the morphology. These findings establish a robust approach to BCN fabrication while revealing dynamic biological interactions that inform nanocarrier design.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"131 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145665093","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}
Pub Date : 2025-12-04DOI: 10.1021/acs.nanolett.5c04416
Joel Henzie
<named-content content-type="pull-quote-attr-maintext" specific-use="quote-only" type="simple"></named-content><named-content content-type="pull-quote-attr-position" specific-use="float" type="simple"></named-content><i>Nano Letters</i> became an important place where our shared idiom of scale took shape. Over 25 years, <i>Nano Letters</i> has chronicled the rise of nanoscience. The journal also holds the peculiar distinction of publishing my first paper as a graduate student. Looking back now, I find myself returning to a few early currents that shaped the field, the journal, and also impacted the arc of my career. In 2002, as a graduate student in an organic chemistry program, I stumbled across a viewpoint article by Professor George Whitesides titled “Self-Assembly at All Scales”. (1) What struck me was not just the topic, but the way the essay transformed “self-assembly” into a shared vocabulary that spanned chemistry, physics, biology, and engineering. It rearranged my thinking: the idea that one principle could provide common ground across such disparate disciplines felt like someone had redrawn the intellectual map I thought I understood. I had also read about George’s “open laboratory” policy, which I took, perhaps naively, as a literal invitation. A few months later, I was in Cambridge, learning from his students and postdocs about soft lithography, microcontact printing, and even the finer points of making espresso. Their quest for simplicity and accessibility in science was compelling: the notion that profound experiments could be carried out with modest, almost improvised tools. That sensibility resonated deeply, and it set me on a different course. Within a few months, I left my organic chemistry program and transferred to Northwestern University in 2003, where I joined the lab of Professor Teri Odom. I began my research in Teri’s group in late 2003, just a few years after the launch of the U.S. National Nanotechnology Initiative (NNI; January 2000) (2) and the debut of <i>Nano Letters</i> (November 2000). (3) At the time, “nanoscience” was still a contested label in some corners of academia, wryly dismissed as clever rebranding or “surface science with better tools”. Yet the act of defining a field by a particular length scale─the nanometer─<i>was</i> radical in the sense that it provided a unifying language that gave the movement visibility and momentum and, just as importantly, offered a common funding target. Suddenly, chemists, physicists, engineers, and biologists could assemble under the same banner, speaking in a shared idiom of scale─a field evolving under a single unit. <i>Nano Letters</i> became an important place where our shared idiom of scale took shape. My first publication appeared in <i>Nano Letters</i> in 2005. (4) The work seems simple by today’s standards, but we were working in newly cleared ground. If you’ll allow me, I’d like to tell a brief story about how those early experiments shaped my career. In that pape
{"title":"Twenty-Five Years along the Nanometer","authors":"Joel Henzie","doi":"10.1021/acs.nanolett.5c04416","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04416","url":null,"abstract":"<named-content content-type=\"pull-quote-attr-maintext\" specific-use=\"quote-only\" type=\"simple\"></named-content><named-content content-type=\"pull-quote-attr-position\" specific-use=\"float\" type=\"simple\"></named-content><i>Nano Letters</i> became an important place where our shared idiom of scale took shape. Over 25 years, <i>Nano Letters</i> has chronicled the rise of nanoscience. The journal also holds the peculiar distinction of publishing my first paper as a graduate student. Looking back now, I find myself returning to a few early currents that shaped the field, the journal, and also impacted the arc of my career. In 2002, as a graduate student in an organic chemistry program, I stumbled across a viewpoint article by Professor George Whitesides titled “Self-Assembly at All Scales”. (1) What struck me was not just the topic, but the way the essay transformed “self-assembly” into a shared vocabulary that spanned chemistry, physics, biology, and engineering. It rearranged my thinking: the idea that one principle could provide common ground across such disparate disciplines felt like someone had redrawn the intellectual map I thought I understood. I had also read about George’s “open laboratory” policy, which I took, perhaps naively, as a literal invitation. A few months later, I was in Cambridge, learning from his students and postdocs about soft lithography, microcontact printing, and even the finer points of making espresso. Their quest for simplicity and accessibility in science was compelling: the notion that profound experiments could be carried out with modest, almost improvised tools. That sensibility resonated deeply, and it set me on a different course. Within a few months, I left my organic chemistry program and transferred to Northwestern University in 2003, where I joined the lab of Professor Teri Odom. I began my research in Teri’s group in late 2003, just a few years after the launch of the U.S. National Nanotechnology Initiative (NNI; January 2000) (2) and the debut of <i>Nano Letters</i> (November 2000). (3) At the time, “nanoscience” was still a contested label in some corners of academia, wryly dismissed as clever rebranding or “surface science with better tools”. Yet the act of defining a field by a particular length scale─the nanometer─<i>was</i> radical in the sense that it provided a unifying language that gave the movement visibility and momentum and, just as importantly, offered a common funding target. Suddenly, chemists, physicists, engineers, and biologists could assemble under the same banner, speaking in a shared idiom of scale─a field evolving under a single unit. <i>Nano Letters</i> became an important place where our shared idiom of scale took shape. My first publication appeared in <i>Nano Letters</i> in 2005. (4) The work seems simple by today’s standards, but we were working in newly cleared ground. If you’ll allow me, I’d like to tell a brief story about how those early experiments shaped my career. In that pape","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"216 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145665094","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}
Pub Date : 2025-12-04DOI: 10.1021/acs.nanolett.5c04822
Sergei Lepeshov, Daniel Alec Farbowitz, Thor August Schimmell Weis, Bingrui Lu, Babak Vosoughi Lahijani, Mikkel Heuck, Søren Stobbe
We present the design, fabrication, and characterization of tunable waveguide-coupled silicon bowtie cavities with strong spatial electromagnetic field confinement. We use nanoelectromechanical in-plane actuation for the tuning, as this combines cryocompatibility with ultralow power consumption. Our device leverages a mode volume below 0.2 cubic wavelengths in the material to reach theoretical Purcell factors above 6,500 and waveguide-coupling efficiency above 30% across the full experimentally measured spectral-tuning range of 11 nm. Our spectral measurements demonstrate reversible tuning of bowtie cavities, and we directly show the in-plane actuation using in situ characterization in a scanning electron microscope. Our results constitute the first demonstration of a low-loss tunable bowtie nanocavity with strong light confinement. This solves a key issue for experiments on strong light-matter interactions for cavity quantum electrodynamics and scalable photonic quantum technologies.
{"title":"Nanoelectromechanical Spectral Control of Silicon Bowtie Nanocavities for Quantum Light Sources","authors":"Sergei Lepeshov, Daniel Alec Farbowitz, Thor August Schimmell Weis, Bingrui Lu, Babak Vosoughi Lahijani, Mikkel Heuck, Søren Stobbe","doi":"10.1021/acs.nanolett.5c04822","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04822","url":null,"abstract":"We present the design, fabrication, and characterization of tunable waveguide-coupled silicon bowtie cavities with strong spatial electromagnetic field confinement. We use nanoelectromechanical in-plane actuation for the tuning, as this combines cryocompatibility with ultralow power consumption. Our device leverages a mode volume below 0.2 cubic wavelengths in the material to reach theoretical Purcell factors above 6,500 and waveguide-coupling efficiency above 30% across the full experimentally measured spectral-tuning range of 11 nm. Our spectral measurements demonstrate reversible tuning of bowtie cavities, and we directly show the in-plane actuation using in situ characterization in a scanning electron microscope. Our results constitute the first demonstration of a low-loss tunable bowtie nanocavity with strong light confinement. This solves a key issue for experiments on strong light-matter interactions for cavity quantum electrodynamics and scalable photonic quantum technologies.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"56 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145674563","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}
Pub Date : 2025-12-04DOI: 10.1021/acs.nanolett.5c05072
Zhaomeng Wang, Li Zhang, Puyue Xia, Wenhao Zhang, Sining Fan, Shaolong Tang
Electrical interconnection of high-density and flexible devices via conductive microparticles represents an effective solution. Achieving stable, low-resistance interfaces critically requires controlled conductive particle deformation during compression. However, conventional metal-coated polymer microspheres typically exhibit a deformation limit of ∼60%. Exceeding this threshold leads to shell fracture and sharply increased contact resistance, severely limiting conductivity. Here, we present self-supporting porous silver microspheres (PAg-MS) with an enhanced deformability and lower contact resistance. PAg-MS are synthesized via liquid–solid interfacial nonwetting spheroidization and dealloying. Nanoindentation experiments and theoretical calculations show that PAg-MS (porosity ≈ 51%) gradually densifies during compression and achieves high deformation exceeding 80%. This significantly increases the electrode contact area, shortens the conductive path, and reduces contact resistance to 0.023 Ω mm2. Reliable LED array interconnections are demonstrated on both rigid and flexible substrates, highlighting the versatility of PAg-MS in diverse electronic systems.
{"title":"Self-Supporting Porous Silver Microspheres with Large Deformability for Low-Resistance Interconnection in Flexible Electronics","authors":"Zhaomeng Wang, Li Zhang, Puyue Xia, Wenhao Zhang, Sining Fan, Shaolong Tang","doi":"10.1021/acs.nanolett.5c05072","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c05072","url":null,"abstract":"Electrical interconnection of high-density and flexible devices via conductive microparticles represents an effective solution. Achieving stable, low-resistance interfaces critically requires controlled conductive particle deformation during compression. However, conventional metal-coated polymer microspheres typically exhibit a deformation limit of ∼60%. Exceeding this threshold leads to shell fracture and sharply increased contact resistance, severely limiting conductivity. Here, we present self-supporting porous silver microspheres (PAg-MS) with an enhanced deformability and lower contact resistance. PAg-MS are synthesized via liquid–solid interfacial nonwetting spheroidization and dealloying. Nanoindentation experiments and theoretical calculations show that PAg-MS (porosity ≈ 51%) gradually densifies during compression and achieves high deformation exceeding 80%. This significantly increases the electrode contact area, shortens the conductive path, and reduces contact resistance to 0.023 Ω mm<sup>2</sup>. Reliable LED array interconnections are demonstrated on both rigid and flexible substrates, highlighting the versatility of PAg-MS in diverse electronic systems.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"115 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145674565","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}
Metal-organic frameworks (MOFs) have emerged as hydroxide conductors for alkaline membrane fuel cells due to their porosity, designability, and ease of functionalization. However, related frameworks, especially single OH- conductive MOFs, are rarely reported because it is difficult to simultaneously balance efficient hydroxide conductivity and high base stability. We synthesized a stable hydroxide ion conductor, [Zr6(μ3-O)4(μ3-OH)4(Meim-BDC)6](OH-)6 [Meim(OH-)-UiO-66 or SXE-6, where SXE = Shanxi electrolyte and Meim-H2BDC = 2-(methylimidazol-1-yl)terephthalic acid], through quaterization of N atoms and subsequent ion exchange of [Zr6(μ3-O)4(μ3-OH)4(Im-BDC)6] [Im-UiO-66, where Im-H2BDC = 2-(imidazol-1-yl)terephthalic acid]. Compared to the original neutral network material, the conductivity of the modified material is increased by 10 times, up to 3.44 mS cm-1 at 80 °C and 99% relative humidity. It should be pointed out that Meim(OH-)-UiO-66 represents the single OH- conductor with the highest conductivity in pure MOFs. What is more, a conductive mechanism is visually exhibited by molecular dynamics simulation, suggesting Grotthuss-like migration in void spaces.
{"title":"Single-Anion Conductor Enabled by Quaterization and Ion Exchange in an Imidazole-Modified Metal-Organic Framework.","authors":"Peng Zhao,Lian-Hong Chen,Jian-Qiang Shen,Hui Gao,Ling Yu,Tian-Tian Zhao,Xian-Ming Zhang","doi":"10.1021/acs.nanolett.5c04368","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04368","url":null,"abstract":"Metal-organic frameworks (MOFs) have emerged as hydroxide conductors for alkaline membrane fuel cells due to their porosity, designability, and ease of functionalization. However, related frameworks, especially single OH- conductive MOFs, are rarely reported because it is difficult to simultaneously balance efficient hydroxide conductivity and high base stability. We synthesized a stable hydroxide ion conductor, [Zr6(μ3-O)4(μ3-OH)4(Meim-BDC)6](OH-)6 [Meim(OH-)-UiO-66 or SXE-6, where SXE = Shanxi electrolyte and Meim-H2BDC = 2-(methylimidazol-1-yl)terephthalic acid], through quaterization of N atoms and subsequent ion exchange of [Zr6(μ3-O)4(μ3-OH)4(Im-BDC)6] [Im-UiO-66, where Im-H2BDC = 2-(imidazol-1-yl)terephthalic acid]. Compared to the original neutral network material, the conductivity of the modified material is increased by 10 times, up to 3.44 mS cm-1 at 80 °C and 99% relative humidity. It should be pointed out that Meim(OH-)-UiO-66 represents the single OH- conductor with the highest conductivity in pure MOFs. What is more, a conductive mechanism is visually exhibited by molecular dynamics simulation, suggesting Grotthuss-like migration in void spaces.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145664200","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}
Pub Date : 2025-12-04DOI: 10.1021/acs.nanolett.5c04315
Neng Ye, Zhaoyu Lu, Junzhe Yang, Junyan Wang, Yangyang Gao, Jingchao Li, Yonglai Lu
Thermal interface materials (TIMs) are essential for enhancing interfacial heat transfer, yet achieving both high through-plane thermal conductivity (κ⊥) and structural conformability remains difficult. This study introduces a vitrimer-based TIM using a diglycidyl-ether end-capped liquid polysulfide prepolymer (EPS), where stress relaxation from dynamic covalent bonds improves interfacial contact. A vertically aligned graphite composite (VAGC) with high κ⊥ (15.5 W m–1 K–1) was fabricated via a combined hot-pressing and “stacking-welding” method. Driven by unstable dynamics from a reversible topological network and high surface free energy of thermodynamic properties, VAGC exhibits spontaneous contact behavior. Under zero pressure, the contact thermal resistance drops sharply at 80–100 °C and reaches 16.4 mm2 K W–1, while the effective thermal conductivity of VAGC reaches 14.4 W m–1 K–1. It is believed that the novel EPS vitrimer offers a promising polymer matrix for advanced TIMs.
热界面材料（TIMs）对于增强界面传热至关重要，但实现高透面导热系数（κ⊥）和结构一致性仍然很困难。本研究介绍了一种基于玻璃聚合体的TIM，它使用了端封二缩水甘油醚的液态聚硫预聚物（EPS），其中动态共价键的应力松弛改善了界面接触。通过热压和“堆叠焊接”相结合的方法制备了具有高κ⊥(15.5 W m-1 K-1)的垂直排列石墨复合材料（VAGC）。在可逆拓扑网络的不稳定动力学和高表面自由能的热力学性质的驱动下，VAGC表现出自发接触行为。零压下，接触热阻在80-100℃时急剧下降，达到16.4 mm2 K W - 1，而VAGC的有效导热系数达到14.4 W m-1 K - 1。认为这种新型EPS聚合物为先进的TIMs提供了一种很有前途的聚合物基体。
{"title":"Low Contact Thermal Resistance without Packaging Pressure in Highly Thermally Conductive Interface Materials Enabled by Polysulfide Vitrimer","authors":"Neng Ye, Zhaoyu Lu, Junzhe Yang, Junyan Wang, Yangyang Gao, Jingchao Li, Yonglai Lu","doi":"10.1021/acs.nanolett.5c04315","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04315","url":null,"abstract":"Thermal interface materials (TIMs) are essential for enhancing interfacial heat transfer, yet achieving both high through-plane thermal conductivity (κ<sub>⊥</sub>) and structural conformability remains difficult. This study introduces a vitrimer-based TIM using a diglycidyl-ether end-capped liquid polysulfide prepolymer (EPS), where stress relaxation from dynamic covalent bonds improves interfacial contact. A vertically aligned graphite composite (VAGC) with high κ<sub>⊥</sub> (15.5 W m<sup>–1</sup> K<sup>–1</sup>) was fabricated via a combined hot-pressing and “stacking-welding” method. Driven by unstable dynamics from a reversible topological network and high surface free energy of thermodynamic properties, VAGC exhibits spontaneous contact behavior. Under zero pressure, the contact thermal resistance drops sharply at 80–100 °C and reaches 16.4 mm<sup>2</sup> K W<sup>–1</sup>, while the effective thermal conductivity of VAGC reaches 14.4 W m<sup>–1</sup> K<sup>–1</sup>. It is believed that the novel EPS vitrimer offers a promising polymer matrix for advanced TIMs.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"21 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145674561","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}
Designing electrocatalysts with high catalytic activity and strong adsorption capacity is crucial for overcoming the key challenges in lithium–sulfur batteries. In this paper, a nitrogen-functionalized MXene loaded with cobalt nanoparticles is prepared via a fluoride-free molten salt etching method. The N-functional groups were introduced via an in situ substitution strategy, while maintaining the layered character of MXene. The resulting cobalt nanoparticles from the etching process were retained in the composite, synergizing with nitrogen to enhance the chemical anchoring of polysulfides and accelerate the redox reaction kinetics. Electrochemical tests demonstrate that Co/N-MX exhibits outstanding catalytic ability and adsorption capacity. Benefiting from the synergistic effect, lithium–sulfur batteries with a Co/N-MX modified separator exhibit improved electrochemical performance. Importantly, this strategy can be extended to other metals such as Cu, Fe, and Ni, with nitrogen functional groups simultaneously introduced onto the MXene surface, demonstrating its versatility and broad applicability.
{"title":"Rational Design of Ultrafine Co, Fe, Ni, and Cu on Fluorine-Free Nitrogen-Doped MXene via a Molten Salt Etching Strategy for the Adsorption–Barrier–Catalyst Functions of Polysulfides toward High-Energy Lithium–Sulfur Batteries","authors":"Zhengran Wang, Fangbing Dong, Liwen Tan, Shenglin Xiong, Jinkui Feng","doi":"10.1021/acs.nanolett.5c04418","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04418","url":null,"abstract":"Designing electrocatalysts with high catalytic activity and strong adsorption capacity is crucial for overcoming the key challenges in lithium–sulfur batteries. In this paper, a nitrogen-functionalized MXene loaded with cobalt nanoparticles is prepared via a fluoride-free molten salt etching method. The N-functional groups were introduced via an in situ substitution strategy, while maintaining the layered character of MXene. The resulting cobalt nanoparticles from the etching process were retained in the composite, synergizing with nitrogen to enhance the chemical anchoring of polysulfides and accelerate the redox reaction kinetics. Electrochemical tests demonstrate that Co/N-MX exhibits outstanding catalytic ability and adsorption capacity. Benefiting from the synergistic effect, lithium–sulfur batteries with a Co/N-MX modified separator exhibit improved electrochemical performance. Importantly, this strategy can be extended to other metals such as Cu, Fe, and Ni, with nitrogen functional groups simultaneously introduced onto the MXene surface, demonstrating its versatility and broad applicability.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"33 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658005","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}
Pub Date : 2025-12-03DOI: 10.1021/acs.nanolett.5c04295
Abraham Kasa,Lakshman Sundar Arumugam,Anja Vanleenhove,Vishal Jose,Thierry Conard,Daniely Santos,Jan D'Haen,Angelica Simbula,Laurence Lutsen,Javier E Durantini,Sixto Giménez,Guy Brammertz,Sudhanshu Shukla,Bart Vermang
Carbon nitride (CN) has emerged as a promising metal-free semiconductor for photoelectrochemical (PEC) water-splitting applications. However, its practical implementation is hindered by low photoactivity compared with inorganic photoanodes. We report the excellent photoactivity of modified CN photoanodes for PEC water oxidation. Incorporating powder precursors during the synthesis induces favorable morphological modifications, enhanced layer ordering, and charge transfer. The powder thiourea-assisted growth of CN boosted the photocurrent by almost 3-fold. This enhancement is attributed to suppressed carrier recombination, improved charge transfer, and the formation of CN and SnS2 heterojunctions. The champion CN photoanode achieved an excellent charge extraction efficiency of up to 69% and a benchmark photocurrent density with and without a hole scavenger of about 2.7 and 2 mA cm-2, respectively for water oxidation at 1.23 V versus RHE in neutral 0.1 M Na2SO4 solution, with an onset potential of 0.32 V vs RHE and external quantum yield reaching 42% at 440 nm.
氮化碳（CN）是一种很有前途的无金属半导体，可用于光电化学（PEC）水分解。然而，与无机光阳极相比，其光活性较低，阻碍了其实际实施。本文报道了改性CN光阳极在PEC水氧化中的优异光活性。在合成过程中加入粉末前体诱导了有利的形态改变，增强了层的有序性和电荷转移。粉末硫脲辅助生长的CN光电流提高了近3倍。这种增强归因于抑制载流子重组，改善电荷转移以及CN和SnS2异质结的形成。在中性0.1 M Na2SO4溶液中，在1.23 V / RHE条件下氧化时，CN光阳极的电荷提取效率高达69%，基准光电流密度分别约为2.7和2 mA cm-2，起始电位为0.32 V / RHE，在440 nm处的外量子产率达到42%。
{"title":"Precursor-Driven Reconfiguration of Bulk and Interface Enhances the Solar-Driven Water-Splitting Performance of Carbon Nitride Photoanode.","authors":"Abraham Kasa,Lakshman Sundar Arumugam,Anja Vanleenhove,Vishal Jose,Thierry Conard,Daniely Santos,Jan D'Haen,Angelica Simbula,Laurence Lutsen,Javier E Durantini,Sixto Giménez,Guy Brammertz,Sudhanshu Shukla,Bart Vermang","doi":"10.1021/acs.nanolett.5c04295","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04295","url":null,"abstract":"Carbon nitride (CN) has emerged as a promising metal-free semiconductor for photoelectrochemical (PEC) water-splitting applications. However, its practical implementation is hindered by low photoactivity compared with inorganic photoanodes. We report the excellent photoactivity of modified CN photoanodes for PEC water oxidation. Incorporating powder precursors during the synthesis induces favorable morphological modifications, enhanced layer ordering, and charge transfer. The powder thiourea-assisted growth of CN boosted the photocurrent by almost 3-fold. This enhancement is attributed to suppressed carrier recombination, improved charge transfer, and the formation of CN and SnS2 heterojunctions. The champion CN photoanode achieved an excellent charge extraction efficiency of up to 69% and a benchmark photocurrent density with and without a hole scavenger of about 2.7 and 2 mA cm-2, respectively for water oxidation at 1.23 V versus RHE in neutral 0.1 M Na2SO4 solution, with an onset potential of 0.32 V vs RHE and external quantum yield reaching 42% at 440 nm.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"4 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145664302","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}
Dirac surface states in a topological insulator (TI) with proximity-induced superconductivity offer a promising platform for realizing Majorana physics. In this work, we demonstrate gate-tunable ambipolar Josephson current in lateral Josephson junction (JJ) devices based on bulk-insulating (Bi,Sb)2Te3 thin films grown by molecular beam epitaxy (MBE). For thinner films, the supercurrent exhibits pronounced gate-tunable ambipolar behavior and is significantly suppressed as the chemical potential approaches the Dirac point yet persists across it. In contrast, thicker films exhibit a much weaker ambipolar response. Moreover, we find that the supercurrent becomes significantly less resilient to external magnetic fields when the chemical potential is tuned near the Dirac point. By performing numerical simulations, we attribute the asymmetric supercurrent observed in thicker TI films to the coexistence of Dirac surface states and bulk conduction channels. The demonstration of gate-tunable ambipolar Josephson transport establishes a foundation for the future exploration of electrically tunable Majorana modes.
{"title":"Gate-Tunable Ambipolar Josephson Current in a Topological Insulator","authors":"Bomin Zhang, Xiaoda Liu, Junjie Qi, Ling-Jie Zhou, Deyi Zhuo, Han Tay, Hongtao Rong, Annie G. Wang, Zhiyuan Xi, Chao-Xing Liu, Chui-Zhen Chen, Cui-Zu Chang","doi":"10.1021/acs.nanolett.5c04854","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c04854","url":null,"abstract":"Dirac surface states in a topological insulator (TI) with proximity-induced superconductivity offer a promising platform for realizing Majorana physics. In this work, we demonstrate gate-tunable ambipolar Josephson current in lateral Josephson junction (JJ) devices based on bulk-insulating (Bi,Sb)<sub>2</sub>Te<sub>3</sub> thin films grown by molecular beam epitaxy (MBE). For thinner films, the supercurrent exhibits pronounced gate-tunable ambipolar behavior and is significantly suppressed as the chemical potential approaches the Dirac point yet persists across it. In contrast, thicker films exhibit a much weaker ambipolar response. Moreover, we find that the supercurrent becomes significantly less resilient to external magnetic fields when the chemical potential is tuned near the Dirac point. By performing numerical simulations, we attribute the asymmetric supercurrent observed in thicker TI films to the coexistence of Dirac surface states and bulk conduction channels. The demonstration of gate-tunable ambipolar Josephson transport establishes a foundation for the future exploration of electrically tunable Majorana modes.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"2 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658006","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}
Pub Date : 2025-12-03DOI: 10.1021/acs.nanolett.5c05437
Nolan Lassaline, Camilla H. Sørensen, Giulia Meucci, Sander J. Linde, Kian Latifi Yaghin, Magnus V. Nielsen, Tuan K. Chau, Damon J. Carrad, Peter Bøggild, Thomas S. Jespersen, Timothy J. Booth
Two-dimensional (2D) materials, such as graphene and hexagonal boron nitride (hBN), provide a versatile platform for quantum electronics. Experiments generally require encapsulation of graphene within hBN flakes, forming a protective van der Waals (vdW) heterostructure that preserves the delicate properties of the embedded crystal. To produce functional devices, heterostructures are typically shaped by electron beam lithography and etching, which have driven progress in 2D materials research. However, patterns are primarily restricted to in-plane geometries such as boxes, holes, and stripes, limiting opportunities for advanced architectures. Here, we use thermal scanning-probe lithography to produce smooth topographic landscapes in vdW heterostructures by patterning the thickness of the top hBN flake with nanometer precision. We electrically gate a sinusoidal topography to impose a periodic electric-field gradient on the graphene layer to spatially modulate charge-carrier density. We observe signatures of the landscape in transport measurements─resistance-peak spreading and commensurability oscillations─establishing this approach for tailoring mathematically precise potentials in quantum electronics.
{"title":"Gradient Electronic Landscapes in van der Waals Heterostructures","authors":"Nolan Lassaline, Camilla H. Sørensen, Giulia Meucci, Sander J. Linde, Kian Latifi Yaghin, Magnus V. Nielsen, Tuan K. Chau, Damon J. Carrad, Peter Bøggild, Thomas S. Jespersen, Timothy J. Booth","doi":"10.1021/acs.nanolett.5c05437","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c05437","url":null,"abstract":"Two-dimensional (2D) materials, such as graphene and hexagonal boron nitride (hBN), provide a versatile platform for quantum electronics. Experiments generally require encapsulation of graphene within hBN flakes, forming a protective van der Waals (vdW) heterostructure that preserves the delicate properties of the embedded crystal. To produce functional devices, heterostructures are typically shaped by electron beam lithography and etching, which have driven progress in 2D materials research. However, patterns are primarily restricted to in-plane geometries such as boxes, holes, and stripes, limiting opportunities for advanced architectures. Here, we use thermal scanning-probe lithography to produce smooth topographic landscapes in vdW heterostructures by patterning the thickness of the top hBN flake with nanometer precision. We electrically gate a sinusoidal topography to impose a periodic electric-field gradient on the graphene layer to spatially modulate charge-carrier density. We observe signatures of the landscape in transport measurements─resistance-peak spreading and commensurability oscillations─establishing this approach for tailoring mathematically precise potentials in quantum electronics.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145665174","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}
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