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Field-Free Spin–Orbit Torque Switching of Canted van der Waals Magnets
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c16826
Bing Zhao, Lalit Pandey, Khadiza Ali, Erdi Wang, Craig M. Polley, Balasubramanian Thiagarajan, Peter Makk, Marcos H. D. Guimarães, Saroj Prasad Dash
{"title":"Field-Free Spin–Orbit Torque Switching of Canted van der Waals Magnets","authors":"Bing Zhao, Lalit Pandey, Khadiza Ali, Erdi Wang, Craig M. Polley, Balasubramanian Thiagarajan, Peter Makk, Marcos H. D. Guimarães, Saroj Prasad Dash","doi":"10.1021/acsnano.4c16826","DOIUrl":"https://doi.org/10.1021/acsnano.4c16826","url":null,"abstract":"Spin–orbit torque (SOT) magnetization switching is crucial for next-generation energy-efficient spintronic technologies. The recent discovery of van der Waals (vdW) magnets holds promise for such SOT phenomena because of their tunable magnetic properties. However, a demonstration of energy-efficient and field-free SOT switching of vdW magnets is required for their potential applications. Here, we demonstrate field-free and deterministic switching using an intrinsic canted vdW magnet Fe<sub>5</sub>GeTe<sub>2</sub> in a heterostructure with Pt having a larger spin Hall conductivity up to room temperature. Using anomalous Hall electrical detection for magnetization readout, we reveal that field-free deterministic SOT switching in the Fe<sub>5</sub>GeTe<sub>2</sub>/Pt Hall devices can be attributed to the canted magnetic anisotropy of Fe<sub>5</sub>GeTe<sub>2</sub>, originating from its crystal and magnetic structures. Detailed second harmonic Hall measurements exhibit a high spin Hall conductivity σ<i><sub>SH</sub></i> ∼ 3 × 10<sup>5</sup>ℏ/2<i>e</i> Ω<sup>–1</sup>m<sup>–1</sup> with an SOT effective damping-like field of 0.06 mT per MA/cm<sup>2</sup>. These findings reveal efficient and field-free SOT phenomena in the canted vdW magnet Fe<sub>5</sub>GeTe<sub>2</sub> up to room temperature and highlight their usefulness in spintronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"103 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nanocomposite Hydrogels and Micro/Nanostructures for Printing Organoids.
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c17587
Daixi Xie, Bingda Chen, Wenqing Wang, Wenjing Guo, Zhiyuan Sun, Long Wang, Bin Shi, Yanlin Song, Meng Su
{"title":"Nanocomposite Hydrogels and Micro/Nanostructures for Printing Organoids.","authors":"Daixi Xie, Bingda Chen, Wenqing Wang, Wenjing Guo, Zhiyuan Sun, Long Wang, Bin Shi, Yanlin Song, Meng Su","doi":"10.1021/acsnano.4c17587","DOIUrl":"https://doi.org/10.1021/acsnano.4c17587","url":null,"abstract":"<p><p>Organoids are 3D artificial miniature organs composed of a cluster of self-renewing and self-organizing cells <i>in vitro</i>, which mimic the functions of real organs. Nanotechnologies, including the preparation of nanomaterials and the fabrication of micro/nanostructures, have been proven to promote cell proliferation, guide cell differentiation, and regulate cell self-organization, showing great promise in engineering organoids. In this Perspective, different types of nanocomposite hydrogels for organoid culture are summarized, the effects of micro/nanostructures on organoid growth and development are discussed, and 3D bioprinting technologies for constructing organoid models are introduced.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reactive Molecular Beam Epitaxy Growth of a 1T-FeS2 Single-Layer-Atomic Structure, Moiré, and Decoupling via Intercalation.
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c17873
Mahesh Krishna Prabhu, Philippe David, Valérie Guisset, Lucio Martinelli, Johann Coraux, Gilles Renaud
{"title":"Reactive Molecular Beam Epitaxy Growth of a 1T-FeS<sub>2</sub> Single-Layer-Atomic Structure, Moiré, and Decoupling via Intercalation.","authors":"Mahesh Krishna Prabhu, Philippe David, Valérie Guisset, Lucio Martinelli, Johann Coraux, Gilles Renaud","doi":"10.1021/acsnano.4c17873","DOIUrl":"https://doi.org/10.1021/acsnano.4c17873","url":null,"abstract":"<p><p>Two-dimensional (2D) iron disulfide (FeS<sub>2</sub>), in its 1<i>T</i> polymorph, is a promising candidate for high-Curie-temperature ferromagnetic applications. Unlike typical van der Waals materials, FeS<sub>2</sub> lacks a naturally lamellar bulk structure and thus cannot be prepared by exfoliation. Consequently, it exists solely as a synthetic 2D magnet, primarily produced via chemical vapor deposition. Here, we propose an alternative synthesis method: reactive molecular beam epitaxy, where an iron layer predeposited on a Au(111) substrate is sulfurized to form FeS<sub>2</sub>. Structural and compositional analyses of the resulting 2D layer─employing scanning tunneling microscopy, electron diffraction, Auger electron spectroscopy, and synchrotron surface X-ray diffraction─confirm a nominal Fe ratio of 1:2, essential for achieving a high Curie temperature. Modeling and fitting the three-dimensional X-ray diffraction data further reveals that the layer crystallizes in the desired 1<i>T</i> polymorph. This 1<i>T</i>-FeS<sub>2</sub> grown on Au(111) exhibits exceptional crystalline quality, largely surpassing that of other 2D transition metal dichalcogenides epitaxially grown on substrates. In addition, it shows pronounced atomic distortions from an ideal 1<i>T</i> structure, attributed to the strain induced by the substrate to achieve a perfectly commensurate 5 × 5 moiré pattern. The 1<i>T</i>-FeS<sub>2</sub> and moiré atomic structures are fully determined with high accuracy on atomic coordinates. Finally, through Cs intercalation, we demonstrate complete decoupling of the FeS<sub>2</sub> layer from the substrate and the release of heteroepitaxial strains.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pressure-Controlled Nanopipette Sensing in the Asymmetric-Conductivity Configuration
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c16079
Sebastian A. Skaanvik, Xinyu Zhang, Ian J. McPherson, Yuqing Wang, Anne-Kathrine K. Larsen, Steffan M. Sønderskov, Patrick R. Unwin, Tomaso Zambelli, Mingdong Dong
{"title":"Pressure-Controlled Nanopipette Sensing in the Asymmetric-Conductivity Configuration","authors":"Sebastian A. Skaanvik, Xinyu Zhang, Ian J. McPherson, Yuqing Wang, Anne-Kathrine K. Larsen, Steffan M. Sønderskov, Patrick R. Unwin, Tomaso Zambelli, Mingdong Dong","doi":"10.1021/acsnano.4c16079","DOIUrl":"https://doi.org/10.1021/acsnano.4c16079","url":null,"abstract":"Nanopipettes are important tools across diverse disciplines, including biology, physics, and materials science. Precisely controlling their characteristics is crucial for many applications. Recent progress in this endeavor has involved using the asymmetric-conductivity configuration with different electrolyte solutions inside and outside the nanopipette, which can greatly improve nanopipette sensing. However, understanding such measurements remains challenging due to the complex interplay of diffusion, electromigration, and electroosmosis. Here, we systematically explore a fundamental regime of the asymmetric-conductivity configuration where classical ion current rectification due to ion-selective migration is minimized and the effect of electroosmotic flow is maximized. We characterized the current–potential and current–distance relationship and revealed that this experimental configuration exhibits many of the characteristics of traditionally rectifying nanopipettes, such as surface charge sensitivity, while the current response can be understood simply from the rate and direction of solution mixing due to electroosmotic flow. To optimize the sensitivity in the asymmetric-conductivity configuration, we introduced a method that uses external pressure to control the fluid flow rates at the aperture, tuning the local ionic environment <i>in situ</i>.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hot Electron Engineering in Layered Heterojunctions for Efficient Infrared Detection
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c14983
Pushkar Dasika, Patrick Hays, Suchithra Puliyassery, Kenji Watanabe, Takashi Taniguchi, Seth Ariel Tongay, Kausik Majumdar
{"title":"Hot Electron Engineering in Layered Heterojunctions for Efficient Infrared Detection","authors":"Pushkar Dasika, Patrick Hays, Suchithra Puliyassery, Kenji Watanabe, Takashi Taniguchi, Seth Ariel Tongay, Kausik Majumdar","doi":"10.1021/acsnano.4c14983","DOIUrl":"https://doi.org/10.1021/acsnano.4c14983","url":null,"abstract":"Although infrared detection is of high technological and strategic importance, the narrow-bandgap materials used for infrared detection often suffer from poor air stability and pose environmental hazards. Hot electron-based detectors avoid such issues by using conventional wide bandgap semiconductors and exploiting intraband transition. However, hot electron infrared detectors usually suffer from poor quantum efficiency. By photoexciting MoS<sub>2</sub> conduction electrons over a thin barrier layer, here we show that a reversal of the role of the emitter and collector results in a &gt;1000-fold enhancement in the photoresponse compared with a conventional metal/2D semiconductor Schottky diode. We reveal that electron–electron scattering plays a key role in the device performance, which can be effectively tuned by a gate voltage. The photodetector exhibits a nearly flat response up to a measurement wavelength of 1800 nm with a responsivity of 42 mA/W (@1550 nm) at room temperature. We demonstrate an operating frequency of 30 kHz @1550 nm excitation (100 kHz @633 nm). The detector chip is integrated with post-processing electronics in a printed circuit board, making it readily useable for system-level applications─a demonstration of heterogeneous integration of 2D materials with conventional electronics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"58 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
22.1% Carbon-Electrode Perovskite Solar Cells by Spontaneous Passivation and Self-Assembly of Hole-Transport Bilayer.
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c16916
Junjie Tong, Chen Dong, Miaosen Yao, Qichao Wang, Chenlei Shen, Yaxin Yue, Lei Yan, Yueyue Gao, Gentian Yue, Weifeng Zhang, Makhsud I Saidaminov, Furui Tan
{"title":"22.1% Carbon-Electrode Perovskite Solar Cells by Spontaneous Passivation and Self-Assembly of Hole-Transport Bilayer.","authors":"Junjie Tong, Chen Dong, Miaosen Yao, Qichao Wang, Chenlei Shen, Yaxin Yue, Lei Yan, Yueyue Gao, Gentian Yue, Weifeng Zhang, Makhsud I Saidaminov, Furui Tan","doi":"10.1021/acsnano.4c16916","DOIUrl":"https://doi.org/10.1021/acsnano.4c16916","url":null,"abstract":"<p><p>Low-temperature printable carbon-electrode perovskite solar cells (C-PSCs) promise commercially scalable and stable low-cost photovoltaic solutions. However, they suffer from low efficiency due to severe performance losses at the perovskite and carbon interface. Here, we propose a spontaneous interface assembly and passivation strategy based on a P3HT/NiO<sub><i>x</i></sub> hole-transport bilayer by introducing quaternary ammonium bromide surfactants into NiO<sub><i>x</i></sub> nanoparticles, and reveal the significant influences from their alkyl chains. Experimental and theoretical results demonstrate that hexyl trimethylammonium bromide (HTAB), with its optimal alkyl chain length, not only ensures the improved monodispersity and film quality of NiO<sub><i>x</i></sub> nanoparticles but also matches and interacts strongly with P3HT side chains, significantly enhancing the molecular orientation of P3HT for superior electronic contact and efficient hole transport between P3HT and HTAB-NiO<sub><i>x</i></sub>. In addition, the Br<sup>-</sup> ions in HTAB-NiO<sub><i>x</i></sub> spontaneously diffuse into a perovskite film, passivating uncoordinated Pb<sup>2+</sup> or I vacancy defects and inhibiting the formation of metallic Pb<sup>0</sup>. Eventually, the low-temperature printable C-PSCs and modules achieve the highest reported efficiency of 22.1 and 18.0%, respectively; exhibit excellent stability at 80-90% high humidity without encapsulation; and demonstrate long-term operational stability for 500 h under maximum power point tracking conditions, maintaining 94% of the initial efficiency.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modulating Intracellular Autophagy and Macropinocytosis for Increased Neighboring Drug Delivery.
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c18465
Shuaipeng Feng, Qingqing Xu, Bin Liu, Ye He, Luming Song, Qinfu Zhao, Siling Wang
{"title":"Modulating Intracellular Autophagy and Macropinocytosis for Increased Neighboring Drug Delivery.","authors":"Shuaipeng Feng, Qingqing Xu, Bin Liu, Ye He, Luming Song, Qinfu Zhao, Siling Wang","doi":"10.1021/acsnano.4c18465","DOIUrl":"https://doi.org/10.1021/acsnano.4c18465","url":null,"abstract":"<p><p>Neighboring effects provided a valuable direction for in-depth penetration of nanoparticles into tumors. However, the uncontrollable drug transcytosis and limited drug uptake hindered by viscous cancer-associated fibroblasts (CAFs) greatly limit their in-depth penetration. Here, we proposed and demonstrated that intracellular autophagosomes could carry the remaining drugs to neighboring cells, and the enhanced macropinocytosis played a major role in neighboring delivery. To enhance the autophagosome-based neighboring delivery, Ca<sup>2+</sup>-doped polydopamine was prepared to load GLS1 inhibitor CB-839 and modified glutamine (839/CG) for triggering macropinocytosis-based active cells uptake. After Ca<sup>2+</sup>-release caused lysosome damage, 839/CG escaped from lysosomes and hindered the autophagosome maturation. Then, Ca<sup>2+</sup>-induced endoplasmic reticulum oscillations and glutamine starvation both increased and blocked autophagy flow, causing 839/CG-contained autophagosome accumulation. Meanwhile, the tumor increased its macropinocytosis in response to mTOR downregulation-induced glutamine hunger, causing \"the more you eat, the hungrier you get\". After tumor death, the 839/CG-contained autophagosomes were released and actively ingested by neighboring hungry tumor cells through macropinocytosis. Combined with the photothermal effect triggered CAF decrease, neighboring cells repeated the above process for in-depth tumor delivery. Also, immunogenic death enhanced the antigen presentation of DCs and infiltration of T cells, thereby inhibiting tumor growth and lung metastasis.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750253","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Bilayer Microfluidics-Based Elastic Encapsulation Method of Liquid Metal Circuits with Cellular Resolution
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-30 DOI: 10.1021/acsnano.4c18309
Chen Hang, Qingyan Rao, Jialu Wu, Jie Qi, Xingyu Jiang
{"title":"A Bilayer Microfluidics-Based Elastic Encapsulation Method of Liquid Metal Circuits with Cellular Resolution","authors":"Chen Hang, Qingyan Rao, Jialu Wu, Jie Qi, Xingyu Jiang","doi":"10.1021/acsnano.4c18309","DOIUrl":"https://doi.org/10.1021/acsnano.4c18309","url":null,"abstract":"Mechanical mismatches at the microscale between bioelectronics and cells severely hinder the successful acquisition of high-quality and stable electrophysiological signals. Room-temperature liquid metals (EGaIn), which possess a near-zero Young’s modulus, present a promising material for achieving stable conformal contact with biological tissues. However, the fluidity of liquid metals limits the elastic encapsulation of the patterned circuits with cellular resolution. To address this challenge, we develop a bilayer microfluidics-based method to elastically encapsulate a high-resolution electrode array (20 μm) within several minutes (&lt;3 min). The alignment-free method overcomes the limitations of packaging polymers and high-resolution aligners, enabling cost-effective, scalable manufacturing for devices. These electronics exhibit excellent wear resistance, high flexibility (&gt;300% strain), and excellent biocompatibility, facilitating long-term stable interfacing with cardiomyocytes and enabling the collection of high-quality (∼30 dB) cell field potential signals as well as epicardial signals (∼42 dB) from living rat models. This rapid and straightforward encapsulation approach improves the precision and integration of liquid metal-based flexible electronics, holding the promise of high-resolution monitoring and treatment, such as electrophysiological mapping, electrical stimulation, and other therapeutic interventions at the cellular levels.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"2 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Imaging of Hydrated and Living Cells in Transmission Electron Microscope: Summary, Challenges, and Perspectives
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-29 DOI: 10.1021/acsnano.5c00871
Olga Kaczmarczyk, Daria Augustyniak, Andrzej Żak
{"title":"Imaging of Hydrated and Living Cells in Transmission Electron Microscope: Summary, Challenges, and Perspectives","authors":"Olga Kaczmarczyk, Daria Augustyniak, Andrzej Żak","doi":"10.1021/acsnano.5c00871","DOIUrl":"https://doi.org/10.1021/acsnano.5c00871","url":null,"abstract":"Transmission electron microscopy (TEM) is well-known for performing in situ studies in the nanoscale. Hence, scientists took this opportunity to explore the subtle processes occurring in living organisms. Nevertheless, such observations are complex─they require delicate samples kept in the liquid phase, low electron dose, and proper cell viability verification methods. Despite being highly demanding, so-called “live-cell” experiments have seen some degree of success. The presented review consists of an exhaustive literature review on reported “live-cell” studies and associated subjects, including liquid phase imaging, electron radiation interactions with liquids, and methods for cell viability testing. The challenges of modern, reliable research on living organisms are widely explained and discussed, and future perspectives for developing these techniques are presented.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"215 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734392","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dynamics Slowdown Induced by Gas Oversolubility in Nanoconfined Fluids
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-29 DOI: 10.1021/acsnano.4c16967
Linh Ngoc Ho, Anne Lesage, Aaron J. Rossini, David Farrusseng, Benoit Coasne
{"title":"Dynamics Slowdown Induced by Gas Oversolubility in Nanoconfined Fluids","authors":"Linh Ngoc Ho, Anne Lesage, Aaron J. Rossini, David Farrusseng, Benoit Coasne","doi":"10.1021/acsnano.4c16967","DOIUrl":"https://doi.org/10.1021/acsnano.4c16967","url":null,"abstract":"Oversolubility refers to the observation in nanoconfined liquids of significant gas solubilities that largely surpass the bulk solubility. While this thermodynamic effect is now well-documented, its impact on the dynamics of fluids confined in nanoporous materials has not been explored. Yet, by affecting adsorption and wetting at solid/liquid interfaces, oversolubility is expected to be a key phenomenon in separation and catalysis but also in geological applications such as pollutant migration in soils, carbon capture/storage in natural environments, and underground/atmosphere exchanges. Here, we employ atom-scale simulations and NMR experiments to show that gas oversolubility is expected in hydrated nanoporous materials and that it reduces both water and ion diffusivities [by 10% up to 60% depending on thermodynamic conditions]. Despite the complexity of adsorption/transport coupling in such gas/liquid/solid systems, we establish that diffusivities in the presence of small gases such as CO<sub>2</sub>, CH<sub>4</sub> and H<sub>2</sub> can be rationalized by accounting for the increase in the confined fluid viscosity (which is found to be directly linked to the decrease in the free volume accessible to the liquid upon solubilization). Moreover, in agreement with the reported data, by invoking Stokes–Einstein relation between the viscosity and diffusivity, we predict that the dynamics slowdown is identical for the confined water molecules and ionic species. We also show that this oversolubility-induced dynamical effect becomes more pronounced as the strength of the molecular interactions between the solubilized gas and the liquid/solid increases. This approach provides a robust formalism to fluid diffusion in nanoconfined environments subjected to gas solubility and potential oversolubility effects.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"2 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734390","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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