{"title":"The In Situ Assembly of an Equipotential Cathode for Nitrite Enrichment Enabling Electrochemical Nitrate Reduction to N2","authors":"Chenyu Bao, Zhiwen Cheng, Dongting Yue, Jianxing Liang, Jingdong Li, Wenlue Cai, Yushan Chen, Shuxun Chen, Maohong Fan, Jinping Jia, Kan Li","doi":"10.1021/acs.nanolett.5c01401","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01401","url":null,"abstract":"Electrocatalytically reducing NO<sub>3</sub><sup>–</sup> to N<sub>2</sub> is of great significance for environmental remediation and global nitrogen cycling. However, it is currently hindered by low N<sub>2</sub> selectivity since adsorbate N-intermediates are hard to migrate and couple each other during the N–N coupling step. Herein, an in situ assembly strategy was taken to attach Pd@Cu<sub>2</sub>O nanoparticles with CuO nanowire arrays to form an equipotential cathode CuO-Pd@Cu<sub>2</sub>O, which optimized N<sub>2</sub> selectivity to 91%, much higher than that of directly loaded Pd–Cu cathode (55%). Theoretical calculations combined with in situ spectroscopies demonstrated that the equipotential cathode can shield the electric field and enrich NO<sub>2</sub><sup>–</sup> intermediate inside. Meanwhile, a unique reaction pathway was revealed that the enriched NO<sub>2</sub><sup>–</sup> can directly couple with *N and also tune the Pd d-band center, avoiding the hurdles in N–N coupling. The approach here provides a new perspective in cathode design and a mechanistic understanding for the N–N coupling reaction.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dynamic Interplay between Deformability and Activity in Cell Entry of Soft Active Nanoparticles","authors":"Haixiao Wan, Zheng Jiao, Jiaqi Li, Xiaobin Dai, Jianfeng Li, Li-Tang Yan","doi":"10.1021/acs.nanolett.5c01445","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01445","url":null,"abstract":"Deformability has been recognized as a prime important characteristic influencing cellular uptake. But little is known about whether it controls cell–nanoparticle interfaces driven out of equilibrium. Here, we report on soft elastic active nanoparticles whose deformability due to the rigidity regulates the nonequilibrium interaction and dynamics in their endocytosis process. Simulations demonstrate a definitely nonmonotonic feature for the dependence of uptake efficiency on nanoparticle rigidity, in striking contrast to their passive counterpart. There exists a minimum activity for certain cellular uptake, which turns to a larger rigidity for a more vertical orientation of the nanoparticle. We analyze these results by developing analytical theories that reveal the physical origin of various energetic contributions and dissipations governed by the dynamic interplay between nanoparticle deformability and activity. Altogether, the present findings provide new insights into the nonequilibrium physics at cellular interfaces and might be of immediate interest to designing soft systems for the desired biomedical applications.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827267","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}
Nano LettersPub Date : 2025-04-14DOI: 10.1021/acs.nanolett.5c00646
Katelyn A. Kirchner, Sohei Ogasawara, Melbert Jeem, Hiromichi Ohta, Akihiro Suzuki, Hiroo Tajiri, Tomoyuki Koganezawa, Loku Singgappulige Rosantha Kumara, Junji Nishii, John C. Mauro, Yasutaka Matsuo, Madoka Ono
{"title":"Controlling Thermal Conductivity of Amorphous SiOx Films through Structural Engineering Utilizing Single Crystal Substrate Surfaces","authors":"Katelyn A. Kirchner, Sohei Ogasawara, Melbert Jeem, Hiromichi Ohta, Akihiro Suzuki, Hiroo Tajiri, Tomoyuki Koganezawa, Loku Singgappulige Rosantha Kumara, Junji Nishii, John C. Mauro, Yasutaka Matsuo, Madoka Ono","doi":"10.1021/acs.nanolett.5c00646","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00646","url":null,"abstract":"Development of thin films with low thermal conductivity (κ) and high dielectric breakdown strength is essential to engineer insulating materials for electronics packaging and other application domains, such as power electronics. Silica glass (SiO<sub>2</sub>) has extremely high dielectric breakdown strength but a relatively high κ compared to multicomponent silicate glasses. This study reveals that a large and systematic decrease in κ can be obtained by shorter intermediate ordering distances controlled by stronger constraints from the substrate surface atoms. The largest effect on κ is observed for SiO<sub><i>x</i></sub> films on Si substrates, which can reach one-third of the bulk value. The change in ordering is observable by the shift of the main halo measured by grazing incidence X-ray total scattering. The improved understanding of the κ of SiO<sub><i>x</i></sub> films presented herein could enable new materials design for electronic devices including wide-bandgap semiconductors.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"183 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827228","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dynamic Interplay between Deformability and Activity in Cell Entry of Soft Active Nanoparticles","authors":"Haixiao Wan, Zheng Jiao, Jiaqi Li, Xiaobin Dai, Jianfeng Li* and Li-Tang Yan*, ","doi":"10.1021/acs.nanolett.5c0144510.1021/acs.nanolett.5c01445","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01445https://doi.org/10.1021/acs.nanolett.5c01445","url":null,"abstract":"<p >Deformability has been recognized as a prime important characteristic influencing cellular uptake. But little is known about whether it controls cell–nanoparticle interfaces driven out of equilibrium. Here, we report on soft elastic active nanoparticles whose deformability due to the rigidity regulates the nonequilibrium interaction and dynamics in their endocytosis process. Simulations demonstrate a definitely nonmonotonic feature for the dependence of uptake efficiency on nanoparticle rigidity, in striking contrast to their passive counterpart. There exists a minimum activity for certain cellular uptake, which turns to a larger rigidity for a more vertical orientation of the nanoparticle. We analyze these results by developing analytical theories that reveal the physical origin of various energetic contributions and dissipations governed by the dynamic interplay between nanoparticle deformability and activity. Altogether, the present findings provide new insights into the nonequilibrium physics at cellular interfaces and might be of immediate interest to designing soft systems for the desired biomedical applications.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"25 16","pages":"6797–6802 6797–6802"},"PeriodicalIF":9.6,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Field-Free Current-Induced Magnetization Switching of a Room-Temperature van der Waals Magnet for Neuromorphic Computing","authors":"Chenxi Zhou, Zhe Guo, Qifeng Li, Gaojie Zhang, Hao Wu, Jinsen Chen, Rongxin Li, Shuai Zhang, Cuimei Cao, Rui Xiong, Haixin Chang, Long You","doi":"10.1021/acs.nanolett.4c06518","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c06518","url":null,"abstract":"Spin orbit torque (SOT) has become a promising approach to manipulating magnetization switching. The high-quality interface is essentially desired for SOT performance, which is readily acquired by two-dimensional (2D) van der Waals (vdW) materials. Recently, a 2D ferromagnetic material, Fe<sub>3</sub>GaTe<sub>2</sub>, has been discovered to possess an above-room-temperature Curie temperature and strong perpendicular magnetic anisotropy, providing an excellent candidate to build spintronic devices. On the other hand, an external magnetic field is necessary for the SOT-driven deterministic switching, hindering the real applications. Here, we realize field-free SOT switching of Fe<sub>3</sub>GaTe<sub>2</sub> at room temperature. Moreover, inspired by the superiority of 2D materials in 3D heterogeneous integration, we explore the potential in the computing in memory. The artificial synapse function is studied and used in the convolutional neural network, achieving a high-accuracy (∼92.8%) pattern recognition. Our work paves the way for magnetic memory and neuromorphic computing.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"09 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827223","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}
Nano LettersPub Date : 2025-04-14DOI: 10.1021/acs.nanolett.5c00263
Tao Wang, Sergio Salaverría, Fernando Aguilar-Galindo, Javier Besteiro-Sáez, Luis M. Mateo, Paula Angulo-Portugal, Jonathan Rodríguez-Fernández, Dolores Pérez, Martina Corso, Diego Peña, Dimas G. de Oteyza
{"title":"Relating Radical Delocalization, Charge Transfer, and Magnetic Ground State in Acene-Derived Oxyradicals","authors":"Tao Wang, Sergio Salaverría, Fernando Aguilar-Galindo, Javier Besteiro-Sáez, Luis M. Mateo, Paula Angulo-Portugal, Jonathan Rodríguez-Fernández, Dolores Pérez, Martina Corso, Diego Peña, Dimas G. de Oteyza","doi":"10.1021/acs.nanolett.5c00263","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00263","url":null,"abstract":"At the same time that our capabilities to synthesize open-shell carbon-based materials are rapidly growing with the development of on-surface synthesis under vacuum conditions, interest in π-magnetism is rising due to its excellent prospects for potential applications. As a result, increasing efforts are being focused on the detailed understanding of open-shell carbon nanostructures and all of the parameters that determine their spin densities and magnetic ground states. Here we present a facile route to synthesize different open-shell acene derivatives with closely related structures by the addition of functional groups. A systematic comparison allows us to draw conclusions on the role of the functional groups and their number and distribution, as well as on the role of the radical state delocalization in relation with the presence or absence of charge transfer at interfaces, which consequently affects the molecule’s π-magnetism.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"97 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831982","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}
Nano LettersPub Date : 2025-04-14DOI: 10.1021/acs.nanolett.5c0123510.1021/acs.nanolett.5c01235
Xian He, Bohan Deng, Jialiang Lang, Zhichuan Zheng, Zhuting Zhang, Hsiangshun Chang, Yufeng Wu, Chong Yang, Wei Zhao, Ming Lei, Hongyi Liu, Kai Huang* and Hui Wu*,
{"title":"Interfacial-Free-Water-Enhanced Mass Transfer to Boost Current Density of Hydrogen Evolution","authors":"Xian He, Bohan Deng, Jialiang Lang, Zhichuan Zheng, Zhuting Zhang, Hsiangshun Chang, Yufeng Wu, Chong Yang, Wei Zhao, Ming Lei, Hongyi Liu, Kai Huang* and Hui Wu*, ","doi":"10.1021/acs.nanolett.5c0123510.1021/acs.nanolett.5c01235","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01235https://doi.org/10.1021/acs.nanolett.5c01235","url":null,"abstract":"<p >The advancement of water electrolysis highlights the growing importance of electrolyzers capable of operating at high current densities, where mass transfer dynamics plays a crucial role. In the electrode reactions, the interfacial water is a key factor in regulating these dynamics. However, the potential of utilizing interfacial-free water (IFW) to modulate electrode behavior remains underexplored. Herein, we investigate the effect of interfacial water structure on hydrogen evolution reaction (HER) performance across different current density ranges, using designed platinum-coated nickel hydroxide on nickel foam (Pt@Ni(OH)<sub>2</sub>-NF) electrodes. We reveal that with increasing current density, changes in interfacial water structure alter the rate-determining step of the HER. Pt@Ni(OH)<sub>2</sub>-NF exhibited excellent performance in alkaline electrolytes, achieving 1000 mA cm<sup>–2</sup> at 114 mV overpotential. This study provides a novel approach to optimizing alkaline water electrolysis dynamics by enhancing mass transfer, further paving the way for more efficient and energy-saving hydrogen production.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"25 16","pages":"6780–6787 6780–6787"},"PeriodicalIF":9.6,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Phase Modulation of 2D Semiconducting GaTe from Hexagonal to Monoclinic through Layer Thickness Control and Strain Engineering","authors":"Wenzhi Quan, Xinyan Wu, Yujin Cheng, Yue Lu, Qilong Wu, Haoxuan Ding, Jingyi Hu, Jialong Wang, Tong Zhou, Qingqing Ji* and Yanfeng Zhang*, ","doi":"10.1021/acs.nanolett.5c0062610.1021/acs.nanolett.5c00626","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00626https://doi.org/10.1021/acs.nanolett.5c00626","url":null,"abstract":"<p >Phase engineering offers a novel approach to modulate the properties of materials for versatile applications. Two-dimensional (2D) GaTe, an emerging III–VI semiconductor, can exist in hexagonal (<i>h</i>) or monoclinic (<i>m</i>) phases with fascinating phase-dependent properties (e.g., isotropic or anisotropic electrical transport). However, the key factors governing GaTe phases remain obscure. Herein, we achieve phase modulation of GaTe by tuning two previously overlooked factors: layer thickness and strain. The precise layer-controlled synthesis of GaTe from a monolayer (1L) to >10L is achieved via molecular beam epitaxy. A layer-dependent phase transition from <i>h</i>-GaTe (1–5L) to <i>m</i>-GaTe (>10L) is unambiguously unveiled by scanning tunneling microscopy/spectroscopy, driven by system energy minimization according to density functional theory calculations. Local phase transitions from ultrathin <i>h</i>-GaTe to <i>m</i>-GaTe are also obtained via introduced tensile strain. This work clarifies the factors influencing GaTe phases, providing valuable guidance for the phase engineering of other 2D materials toward the desired properties and applications.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"25 16","pages":"6614–6621 6614–6621"},"PeriodicalIF":9.6,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dipole–Dipole Interaction-Induced Direct Self-Assembly of Ag2S Quantum Dots into Supercrystals in Solution","authors":"Ziyan Zhang, Chuncheng Li, Huaiyu Xu, Hongchao Yang, Peng Dai, Yejun Zhang, Jiang Jiang, Fengjia Fan, Zhaochuan Fan, Yuliang Zhao, Qiangbin Wang","doi":"10.1021/acs.nanolett.5c00889","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00889","url":null,"abstract":"Long-range ordered supercrystals (SCs) built up by colloidal nanocrystals (NCs) represent a class of novel metamaterials with unique collective properties. While great attention has been paid to the ligand-controlled assembly of NCs, the contribution of the inorganic core is considered limited because of the weak core–core interactions. Here, we report the spontaneous assembly of Ag<sub>2</sub>S quantum dots (QDs) into three-dimensional SCs in solution, driven by pronounced dipole–dipole interactions. Dielectric spectroscopy shows a large permanent dipole moment of 516.7 D in 4.2 nm Ag<sub>2</sub>S QDs, and multiscale molecular simulation proves the dipole–dipole interaction-driven crystallization of Ag<sub>2</sub>S QDs. Moreover, we demonstrate that tuning the dipole–dipole interactions facilitates the formation of diverse nanostructures, including SCs, nanochains, and monodisperse nanoparticles. These findings offer a straightforward strategy for SC synthesis and establish the dipole–dipole interactions as a key driving force of NC self-assembly with broad implications for colloidal nanomaterials and their emergent functionalities.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"74 5 Pt 1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831983","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}
Nano LettersPub Date : 2025-04-14DOI: 10.1021/acs.nanolett.5c00851
Grégoire Magagnin, Martine Le Berre, Sara Gonzalez, Brice Gautier, Damien Deleruyelle, Bertrand Vilquin, Jordan Bouaziz
{"title":"An Original Positive-Up-Negative-Down Protocol for Electrical Characterization of Antiferroelectric Materials","authors":"Grégoire Magagnin, Martine Le Berre, Sara Gonzalez, Brice Gautier, Damien Deleruyelle, Bertrand Vilquin, Jordan Bouaziz","doi":"10.1021/acs.nanolett.5c00851","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00851","url":null,"abstract":"This work introduces the AFE-PUND measurement method, an original positive up negative down (PUND) protocol intended to accurately study antiferroelectric (AFE) thin-film behavior. As for its FE counterpart, the AFE-PUND method isolates switching currents from nonswitching contributions, enabling a precise extraction of saturation polarization and coercive fields from hysteresis loop curves. In this paper, AFE-PUND was deployed on AFE ZrO<sub>2</sub> films of varying thicknesses. The results reveal that saturation polarization increases with film thickness, indicating enhanced domain stability, while endurance cycles showcase the wake-up effect and its eventual fatigue-induced degradation in thicker films. Similarly, coercive fields decrease with thickness, reflecting reduced switching barriers and a sharper transition between the tetragonal and orthorhombic phases. AFE-PUND establishes itself as an extremely valuable method for advancing the understanding and optimization of AFE materials.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"25 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827231","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}