ACS Nano最新文献

{"title":"Regulation of Reaction Pathways in Coordinated Chains by Directional Mechanical Force","authors":"Zhen Xu, Xin Li, Jie Li, Huamei Chen, Yu Wang, Mingjun Zhong, Shimin Hou, Qian Shen, Xue Zhang, Ziyong Shen, Jing-Tao Lü, Lian-Mao Peng, Kai Wu, Jing Liu, Yajie Zhang, Song Gao, Yongfeng Wang","doi":"10.1021/acsnano.4c13622","DOIUrl":"https://doi.org/10.1021/acsnano.4c13622","url":null,"abstract":"Mechanochemistry refers to chemical reactions induced by mechanical forces. Due to different reaction mechanisms, products obtained through mechanochemistry can be distinct from those produced by thermochemistry and photochemistry. Scanning probe microscopy is a powerful tool for studying single-molecule mechanochemical processes. Mechanical force is a vector that has both magnitude and direction. Previous studies have focused on triggering reactions by forces and measuring their magnitude. In this work, we use the direction of the force to regulate the reaction pathway in a spin-crossover coordinated chain. The chains are prepared via the dehydrogenated coordination reaction between tetrahydroxybenzene molecules and Ni atoms on Au(111). The Ni atoms in the chain alternate between a high-spin state and a low-spin state. By altering Ni–O bond lengths and O–Ni–O angles through the directional mechanical force, a chemical process occurs, and the spin state of Ni undergoes a transition. With the attraction from a Au tip, the Ni atom is pulled from high-spin to low-spin state. With the repulsion from a C₆₀-functionalized tip, the low-spin Ni atom is pushed to the high-spin state. The force to induce the reaction is measured by qPlus atomic force microscopy. This study provides an approach for regulating chemical pathways.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"29 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192690","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":"Pulse Current-Induced Homogeneous Phase Nucleation for High-Performance Conversion-Type Cathodes","authors":"Chuntao Ma, Yuhao Ma, Shuai Li, Hongyu Liu, Hao Wang, Dong Yan, Xiaobin Niu, Hong Li, Liping Wang","doi":"10.1021/acsnano.4c18009","DOIUrl":"https://doi.org/10.1021/acsnano.4c18009","url":null,"abstract":"Conversion-type transition metal-based materials (MZ_<i>x</i>) are considered promising cathodes for lithium metal batteries due to their low cost, abundant availability, and high theoretical energy density. However, they suffer from rapid capacity decay caused by the transformation into two inhomogeneous phases during discharge. Herein, we use a pulse current discharge activation method (under 3C) to induce homogeneous phase nucleations. As a result, the microsized FeS₂ cathode transforms into a homogeneous mixture of nanosized Fe and Li₂S, effectively mitigating volume expansion. It exhibits exceptional cycling performance, delivering a specific capacity of 572.8 mAh g^–1 after 800 cycles at 0.33C. Even at a high areal capacity of 5.4 mAh cm^–2, it undergoes 180 cycles with a capacity retention of 89.3% at 0.33C. This work highlights the crucial role of homogeneous nucleation in achieving long cycling life for conversion-type cathodes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"21 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192693","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":"Nanobody-Mediated Cellular Uptake Maximizes the Potency of Polylysine Dendrimers While Preserving Solid Tumor Penetration","authors":"Daniel Yuen, Orlagh M. Feeney, Leo Noi, Sudhir Shengule, Victoria M. McLeod, Pauline Reitano, Sammi Tsegay, Richard Hufton, Zachary H Houston, Nicholas L. Fletcher, James Humphries, Kristofer J. Thurecht, Carleen Cullinane, David J. Owen, Christopher J.H. Porter, Angus P.R. Johnston","doi":"10.1021/acsnano.4c10851","DOIUrl":"https://doi.org/10.1021/acsnano.4c10851","url":null,"abstract":"Dendrimers are branched macromolecular structures that are useful nanocarriers for small-molecule drugs, such as cancer therapeutics. Their small size permits penetration into solid tumors, coupled with functionalization with a low-fouling PEG coating that minimizes transient cellular interactions and enhances plasma circulation time. While PEGylated dendrimers show significant promise as anticancer therapeutics, there is potential to increase tumor cell specificity and drive uptake of drugs into cells by conjugating cell-targeting ligands onto the dendrimers. To achieve this, we used an expanded genetic code and bio-orthogonal click chemistry to functionalize monomethyl auristatin E (MMAE)-loaded PEGylated dendrimers with a single tumor cell-targeting nanobody per dendrimer. The uniform addition of a single nanobody ligand facilitated greater intracellular uptake of the drug payload into HER2-positive target cells, while preserving the desirable circulatory characteristics of dendrimers. While the nanobody–dendrimer conjugates show similar levels of tumor infiltration over 24 h compared to unmodified dendrimers, the targeted dendrimers had significantly greater inhibition of tumor growth and long-term retention in the tumors. Our results highlight that biodistribution studies alone are poor predictors of therapeutic performance. The controlled conjugation strategy presented here preserves the size advantage and tissue penetration of dendrimers while maximizing targeted cellular uptake and potency in difficult-to-access solid tumor tissue.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"25 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192663","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":"Novel Lithiophilic Silver Selenide Nanocrystals within Porous Carbon Microsphere: Tailoring Pore Structures for Enhanced Lithium Metal Battery Anodes","authors":"Hyo Yeong Seo, Yeong Beom Kim, Thillai Govindaraja Senthamaraikannan, Dong-Hee Lim, Yun Chan Kang, Gi Dae Park","doi":"10.1021/acsnano.4c14290","DOIUrl":"https://doi.org/10.1021/acsnano.4c14290","url":null,"abstract":"To enable the practical use of a lithium metal anode, the rational design of three-dimensional (3D) host materials is considered as a promising approach to mitigate lithium dendrite formation and accommodate substantial volume fluctuations. Herein, we first design a 3D conductive host material comprised of Ag₂Se nanocrystals encapsulated within closed pore structured porous carbon microspheres. The homogeneous distribution of the AgLi alloy and Li₂Se phases, generated through the consecutive conversion and alloying reaction of the Ag₂Se phase, enables the developed host materials to exhibit rapid lithium deposition kinetics. Additionally, the inner void structures with encapsulated lithiophilic nanocrystals promote primary deposition within the carbon framework without dendrite growth. Consequently, optimized pore structure as well as position of lithiophilic nanocrystals in carbon microsphere are rationally tailored for stable plating/stripping behaviors of lithium with high Coulombic efficiency and stable voltage profiles. Paired with the LiNi_0.8Co_0.1Mn_0.1O₂ cathode, the assembled full cell demonstrates outstanding cycling stability and impressive high-rate performance, highlighting its potential for practical applications. Moreover, to explore how different pore structures influence the stability of the Li metal host, Ag₂Se@C hosts with various pore structures (including open pore structures and densely structured configurations without inner voids) are also fabricated and compared with the developed host material.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"46 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192691","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":"Boosting Capacitive Deionization in MoS2 via Interfacial Coordination Bonding and Intercalation-Induced Spacing Confinement","authors":"Xiaosong Gu, Ranhao Wang, Songhe Yang, Yangzi Shangguan, Xuezhen Feng, Hong Chen","doi":"10.1021/acsnano.4c17436","DOIUrl":"https://doi.org/10.1021/acsnano.4c17436","url":null,"abstract":"Capacitive deionization (CDI) is a green and promising technology for seawater desalination, with its capacity and industrial application being severely hindered by efficient electrode materials. Layered molybdenum disulfide (MoS₂) has garnered significant attention for CDI applications, while its performance is hampered by weak surface hydrophilicity, high interfacial resistance, and sluggish electron transport. Herein, we introduce an interfacial and intercalation dual-engineering strategy by covalently functionalizing the hydrophilic pyridine groups within the 1T-MoS₂ layer (Py-MoS₂); an electron-rich interface with an expanded interlayer spacing has been achieved synergistically. A state-of-the-art high desalination capacity of 43.92 mg g^–1 and exceptional cycling stability have been achieved, surpassing all of the reported existing MoS₂-based CDI electrodes. Comprehensive characterization and theoretical modeling reveal that covalently engineered pyridine groups enhance ion affinity via interfacial coordination, accelerate charge transfer, and expand ion-accessible sites within the MoS₂ interlayer spacing through intercalation-induced structural modulation. These synergistic effects dramatically boost the ion adsorption kinetics, mass transfer efficiency, and salt ion uptake capacity within Py-MoS₂ for CDI application. Our work presents an interfacial and intercalation dual-engineering strategy to promote the seawater desalination of 2D materials, paving new insights for next-generation high-performance CDI electrode development.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"134 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124844","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":"Transdisciplinarity: Toward Trans Inclusion and Creative Artistic Expression in the Physical Sciences","authors":"Saxton Fisher*,&nbsp;","doi":"10.1021/acsnano.4c1808410.1021/acsnano.4c18084","DOIUrl":"https://doi.org/10.1021/acsnano.4c18084https://doi.org/10.1021/acsnano.4c18084","url":null,"abstract":"","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 4","pages":"3967–3968 3967–3968"},"PeriodicalIF":15.8,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087927","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":"Deep Learning and Single-Molecule Localization Microscopy Reveal Nanoscopic Dynamics of DNA Entanglement Loci","authors":"Maged F. Serag, Maram Abadi, Hajar Al-Zarah, Omar Ibrahim, Satoshi Habuchi","doi":"10.1021/acsnano.4c15364","DOIUrl":"https://doi.org/10.1021/acsnano.4c15364","url":null,"abstract":"Understanding molecular dynamics at the nanoscale remains challenging due to limitations in the temporal resolution of current imaging techniques. Deep learning integrated with Single-Molecule Localization Microscopy (SMLM) offers opportunities to probe these dynamics. Here, we leverage this integration to reveal entangled polymer dynamics at a fast time scale, which is relatively poorly understood at the single-molecule level. We used Lambda DNA as a model system and modeled their entanglement using the self-avoiding wormlike chain model, generated simulated localizations along the contours, and trained the deep learning algorithm on these simulated images to predict chain contours from sparse localization data. We found that the localizations are heterogeneously distributed along the contours. Our assessments indicated that chain entanglement creates local diffusion barriers for switching buffer molecules, affecting the photoswitching kinetics of fluorescent dyes conjugated to the DNA molecules at discrete DNA segments. Tracking these segments demonstrated stochastic and subdiffusive migration of the entanglement loci. Our approach provides direct visualization of nanoscale polymer dynamics and local molecular environments previously inaccessible to conventional imaging techniques. In addition, our results suggest that the switching kinetics of the fluorophores in SMLM can be used to characterize nanoscopic local environments.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"10 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124843","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":"Nanobiohybrid Oncolytic Bacteria with Optimized Intratumoral Distribution for Combined Sono–Photodynamic/Immunotherapy","authors":"Xu Zhang, Zhongsheng Zang, Zhenguo Liang, Xiaoyu Xu, Jinling Zheng, Na Liang, Shayibai Shabiti, Zixi Wang, Shiwen Yu, Yujue Wang, Chenli Liu, Wenjun Li, Lintao Cai","doi":"10.1021/acsnano.4c16740","DOIUrl":"https://doi.org/10.1021/acsnano.4c16740","url":null,"abstract":"“Living therapeutic carriers” present a promising avenue for cancer research, but it is still challenging to achieve uniform and durable distribution of payloads throughout the solid tumor owing to the tumor microenvironment heterogeneity. Herein, a living drug sprinkle biohybrid (YB1–HCNs) was constructed by hitching acid/enzyme-triggered detachable nanoparticles (HCNs) backpack on the surface of metabolic oligosaccharide-engineered oncolytic bacteria YB1. Along with the process of tumor penetration by bacterial hypoxia navigation, YB1–HCNs responsively and continuously release HCNs, achieving a uniform distribution of loaded agents throughout the tumor. Upon successive irradiation of laser and ultrasound (US), the HCNs can separately generate type II and type I ROS for superior sono–photodynamic therapy (SPDT), which enables HCNs to synergize with YB1 for a satisfactory therapeutic effect in both superficial normoxic and deep hypoxic regions of the tumor. After a single dose, this efficient combination realized 98.3% primary tumor inhibition rate and prolonged survival of mice for 90 days with no recurrence, further inducing a powerful immunological memory effect to completely suppress tumor rechallenge in cured mice. Such a bacterial hybridization vector enables optimization of the spatial distribution of YB1 and HCNs, providing an innovative strategy to maximize therapeutic outcomes and evoke durable antitumor immunity.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083958","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":"Transdisciplinarity: Toward Trans Inclusion and Creative Artistic Expression in the Physical Sciences","authors":"Saxton Fisher","doi":"10.1021/acsnano.4c18084","DOIUrl":"https://doi.org/10.1021/acsnano.4c18084","url":null,"abstract":"This Editorial and the accompanying journal front cover are part of the ACS Diversity &amp; Inclusion Cover Art series that seeks to amplify marginalized voices and recognize groups historically excluded from chemistry, including LGBTQ+ chemists. As a queer and trans scientist, seeing a trans pride flag or a transmission electron microscope (TEM) are both everyday occurrences, but it feels almost shocking to see the two together, because they are thought of as belonging in different spheres. In this drawing titled “Queer at the Nanoscale,” I aimed to illustrate a vision for the inclusion of queer and trans people in chemistry and materials science. Being a PhD candidate working in the field of nanomaterials, I wanted to include objects I work closely with in my research ─ glassware and a TEM (with the green glow of the electron beam on the phosphor screen)─juxtaposed with symbols from the life of people from historically excluded groups. Among this imagery is a pride flag inclusive of trans and intersex people of color, a lab coat with a pronoun button, and a set of forearm crutches. Drawing from my experiences, the piece focuses on queer/trans inclusion while also creating space for representation of people with additional intersecting identities, such as race and disability, because the fight for a seat at the table is a collective and intersectional one. By collecting all these individual objects and imagery together in collage-like fashion, I hope to show these two worlds─that of science and of queer/trans existence─collided into one, giving an abstract depiction of what true equity and belonging might feel like for trans scientists. Also in this scene is an upward-pointing pink triangle with a nitrile-gloved hand raised in a fist of solidarity to center the fact that the liberation of queer/trans people and their full inclusion in STEM fields is an ongoing struggle. The pink triangle is an iconic symbol of the queer community that has been reclaimed from its original inverted orientation as a badge to label gay men in Nazi concentration camps. (1,2) This reclamation began in the 1970s, (1) and the pink triangle later gained traction as the focal point of the iconic SILENCE = DEATH posters used by activists in the AIDS Coalition to Unleash Power (ACT UP) in the 1980s. (3) In my drawing, within the pink triangle sits the transgender symbol as well as the molecular structures of estrogen (right) and testosterone (left), the life-saving hormones that trans people fight for access to. With this work I also draw upon my experience in the visual arts and my ongoing hope to advocate for the merit of creativity and novel visualizations within STEM fields. I believe that it is especially crucial for these aspects of creative artistic expression to be interwoven into scientific practice in a time when interdisciplinary and transdisciplinary approaches (pun intended) are needed to tackle complex 21st century issues. As artists we have a unique perspecti","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"12 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083519","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":"Organic Modulators Enable Morphological Diversity in Colloidal Crystals Engineered with DNA","authors":"Nikhil S. Chellam, Heather A. Calcaterra, Qinsi Xiong, George C. Schatz, Chad A. Mirkin","doi":"10.1021/acsnano.4c17881","DOIUrl":"https://doi.org/10.1021/acsnano.4c17881","url":null,"abstract":"Colloidal crystal engineering with DNA is a powerful way of generating a wide variety of crystals spanning over 90 different symmetries. However, in many cases, crystals with well-defined habits are difficult, if not impossible, to make, in part due to rapid crystal defect formation and propagation. This is especially true in the case of face-centered cubic (FCC) structures. Herein, we report a strategy that uses formamide as a chemical modulator to slow down colloidal crystal growth, which decreases defect formation and yields higher-quality crystals. Formamide forms hydrogen bonds with DNA bases and destabilizes the DNA duplex; in the context of colloidal crystallization, formamide leads to the disassembly of undercoordinated particles (defect architectures) and facilitates their reassembly into structures with the maximum number of nearest-neighbor contacts and DNA bonds. When targeting an FCC lattice comprised of DNA-modified spherical 20 nm particles, formamide promotes the formation of its Wulff polyhedron (a truncated octahedron), never observed before in colloidal crystal engineering with DNA. Importantly, kinetic habits, including tetrahedra, octahedra, icosahedra, and decahedra, are also observed depending on formamide concentration.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"13 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083512","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}