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In Situ Alloying Enabled by Active Liquid Metal Filler for Self-Healing Composite Polymer Electrolytes

Angewandte Chemie 2024年第47期136卷

作者： Dr. Kai Wu Dr. Zhengyu Ju Dr. Bowen Zhang Prof. Amy C. Marschilok Prof. Esther S. Takeuchi Prof. Kenneth J. Takeuchi Prof. Guihua Yu Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin 78712 Austin TX USA Institute of Energy Sustainability Environment and Equity Stony Brook University 11794 Stony Brook NY USA Department of Chemistry Stony Brook University 11794 Stony Brook NY USA Interdisciplinary Science Department Brookhaven National Laboratory 11973 Upton NY USA Department of Materials Science and Chemical Engineering Stony Brook University 11794 Stony Brook NY USA

Solid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces Ga 62.5 In 21.5 Sn 16 (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self-healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li-ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li-LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid-state Li/LiFePO 4 battery achieves promising full-cell functionality with notable rate performance and stable cycle life. This active filler-mediated self-healing approach could bring new insights into the battery design in versatile solid-state systems.

关键词： Solid-state battery Composite polymer electrolyte Liquid metal Lithium-metal battery Li dendrite

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Optical Biosensing: Sensitivity-Enhancing Strategies in Optical Biosensing (Small 4/2021)

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Small 2021年第4期17卷

作者： Youngsun Kim John Gonzales Yuebing Zheng Materials Science and Engineering Program and Texas Materials Institute Walker Department of Mechanical Engineering The University of Texas at Austin Austin TX 78712 USA

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Shape Anisotropy-Governed High-Performance Nanomagnetosol for In Vivo Magnetic Particle Imaging of Lungs

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Small 2024年第5期20卷 2305300-2305300页

作者： Nigam, Saumya Mohapatra, Jeotikanta Makela, Ashley V. Hayat, Hanaan Rodriguez, Jessi Mercedes Sun, Aixia Kenyon, Elizabeth Redman, Nathan A. Spence, Dana Jabin, George Gu, Bin Ashry, Mohamed Sempere, Lorenzo F. Mitra, Arijit Li, Jinxing Chen, Jiahui Wei, Guo-Wei Bolin, Steven Etchebarne, Brett Liu, J. Ping Contag, Christopher H. Wang, Ping Precision Health Program Michigan State University East LansingMI48824 United States Department of Radiology College of Human Medicine Michigan State University East LansingMI48824 United States Department of Physics The University of Texas at Arlington ArlingtonTX76019 United States Michigan State University East LansingMI48824 United States Department of Biomedical Engineering College of Engineering Michigan State University East LansingMI48824 United States Human Biology Program College of Natural Science Michigan State University East LansingMI48824 United States Department of Obstetrics Gynecology and Reproductive Sciences College of Human Medicine Michigan State University East LansingMI48824 United States Department of Materials Science and Engineering National Cheng Kung University Tainan City701 Taiwan Department of Mathematics College of Natural Science Michigan State U niversity East LansingMI48824 United States Department of Electrical and Computer Engineering College of Engineering Michigan State University East LansingMI48824 United States Department of Biochemistry and Molecular Biology College of Natural Science Michigan State University East LansingMI48824 United States Department of Pathobiology and Diagnostic Investigation College of Veterinary Medicine Michigan State University East LansingMI48824 United States Osteopathic Medical Specialties College of Osteopathic Medicine Michigan State University East LansingMI48824 United States Department of Microbiology and Molecular Genetics Michigan State University East LansingMI48824 United States

Caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), coronavirus disease 2019 (COVID-19) has shown extensive lung manifestations in vulnerable individuals, putting lung imaging and monitoring at the forefront of early detection and treatment. Magnetic particle imaging (MPI) is an imaging modality, which can bring excellent contrast, sensitivity, and signal-to-noise ratios to lung imaging for the development of new theranostic approaches for respiratory diseases. Advances in MPI tracers would offer additional improvements and increase the potential for clinical translation of MPI. Here, a high-performance nanotracer based on shape anisotropy of magnetic nanoparticles is developed and its use in MPI imaging of the lung is demonstrated. Shape anisotropy proves to be a critical parameter for increasing signal intensity and resolution and exceeding those properties of conventional spherical nanoparticles. The 0D nanoparticles exhibit a 2-fold increase, while the 1D nanorods have a > 5-fold increase in signal intensity when compared to VivoTrax. Newly designed 1D nanorods displayed high signal intensities and excellent resolution in lung images. A spatiotemporal lung imaging study in mice revealed that this tracer offers new opportunities for monitoring disease and guiding intervention. © 2023 The Authors. Small published by Wiley-VCH GmbH.

关键词： Nanorods

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Machine learning assisted phase and size-controlled synthesis of iron oxides

arXiv

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arXiv 2023年

作者： Liu, Juejing Zhang, Zimeng Li, Xiaoxu Zong, Meirong Wang, Yining Wang, Suyun Chen, Ping Wan, Zaoyan Zhao, Yatong Liu, Lili Liang, Yangang Wang, Wei Wang, Zheming Wang, Shiren Guo, Xiaofeng Saldanha, Emily G. Rosso, Kevin M. Zhang, Xin Physical and Computational Sciences Directorate Pacific Northwest National Laboratory RichlandWA99354 United States Department of Chemistry Washington State University PullmanWA99164 United States Materials Science and Engineering Program Washington State University PullmanWA99164 United States Department of Industrial and Systems Engineering Texas A&M University College StationTX77843 United States Energy and Environment Directorate Pacific Northwest National Laboratory RichlandWA99354 United States National Security Directorate Pacific Northwest National Laboratory RichlandWA99354 United States

The controllable synthesis of iron oxides particles is a critical issue for materials science, energy storage, biomedical applications, environmental science, and earth science. However, synthesis of iron oxides with desired phase and size are still a time-consuming and trial-and-error process. This study presents solutions for two fundamental challenges in materials synthesis: predicting the outcome of a synthesis from specified reaction parameters and correlating sets of parameters to obtain products with desired outcomes. Four machine learning algorithms, including random forest, logistic regression, support vector machine, and k-nearest neighbor, were trained to predict the phase and particle size of iron oxide based on experimental conditions. Among the models, random forest exhibited the best performance, achieving 96% and 81% accuracy when predicting the phase and size of iron oxides in the test dataset. Premutation feature importance analysis shows that most models (except logistic regression) rely on known features such as precursor concentration, pH, and temperature to predict the phases from synthesis conditions. The robustness of the random forest models was further verified by comparing prediction and experimental results based on 24 randomly generated methods in additive and non-additive systems not included in the datasets. The predictions of product phase and particle size from the models are in good agreement with the experimental results. Additionally, a searching and ranking algorithm was developed to recommend potential synthesis parameters for obtaining iron oxide products with desired phase and particle size from previous studies in the dataset. This study lays the foundation for a closed-loop approach in materials synthesis and preparation, from suggesting potential reaction parameters from the dataset and predicting potential outcomes, through conducting experiments and analysis, to enriching the dataset. Copyright © 2023, The Authors. All ri

关键词： Particle size

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Coordination corrected ab initio formation enthalpies

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npj Computational materials 2019年第1期5卷 633-644页

作者： Rico Friedrich Demet Usanmaz Corey Oses Andrew Supka Marco Fornari Marco Buongiorno Nardelli Cormac Toher Stefano Curtarolo Department of Mechanical Engineering and Materials Science Duke UniversityDurhamNC 27708USA Center for Materials Genomics Duke UniversityDurhamNC 27708USA Department of Physics and Science of Advanced Materials Program Central Michigan UniversityMount PleasantMI 48859USA Department of Physics and Department of Chemistry University of North TexasDentonTX 76203USA Materials Science Electrical EngineeringPhysics and ChemistryDuke UniversityDurhamNC 27708USA Fritz-Haber-Institut der Max-Planck-Gesellschaft 14195 Berlin-DahlemGermany

The correct calculation of formation enthalpy is one of the enablers of ab-initio computational materials *** several classes of systems(***)standard density functional theory produces incorrect *** we propose the“coordination corrected enthalpies”method(CCE),based on the number of nearest neighbor cation–anion bonds,and also capable of correcting relative stability of *** uses calculations employing the Perdew,Burke and Ernzerhof(PBE),local density approximation(LDA)and strongly constrained and appropriately normed(SCAN)exchange correlation functionals,in conjunction with a quasiharmonic Debye model to treat zero-point vibrational and thermal *** benchmark,performed on binary and ternary oxides(halides),shows very accurate room temperature results for all functionals,with the smallest mean absolute error of 27(24)meV/atom obtained with *** zero-point vibrational and thermal contributions to the formation enthalpies are small and with different signs—largely canceling each other.

关键词： corrected vibrational oxides

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Li2S6-Integrated PEO-Based Polymer Electrolytes for All-Solid-State Lithium-Metal Batteries

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Angewandte Chemie 2021年第32期133卷

作者： Dr. Ruyi Fang Dr. Biyi Xu Nicholas S. Grundish Dr. Yang Xia Dr. Yutao Li Chengwei Lu Dr. Yijie Liu Dr. Nan Wu Prof. John B. Goodenough Materials Science and Engineering Program and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

The integration of Li 2 S 6 within a poly(ethylene oxide) (PEO)-based polymer electrolyte is demonstrated to improve the polymer electrolyte's ionic conductivity because the strong interplay between O 2− (PEO) and Li + from Li 2 S 6 reduces the crystalline volume within the PEO. The Li/electrolyte interface is stabilized by the in situ formation of an ultra-thin Li 2 S/Li 2 S 2 layer via the reaction between Li 2 S 6 and lithium metal, which increases the ionic transport at the interface and suppresses lithium dendrite growth. A symmetric Li/Li cell with the Li 2 S 6 -integrated composite electrolyte has excellent cyclability and a high critical current density of 0.9 mA cm −2 at 40 °C. Impressive electrochemical performance is demonstrated with all-solid-state Li/LiFePO 4 and high-voltage Li/LiNi 0.8 Mn 0.1 Co 0.1 O 2 cells at 40 °C.

关键词： all-solid-state battery composite electrolyte Li+ conductivity Li2S6 poly(ethylene oxide)

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Quantifying the Response of Diverse Nanoparticles Towards Laser-Induced Thermoelectric Field to Enhance Applications in Nanorobotics

Quantifying the Response of Diverse Nanoparticles Towards La...

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IEEE Photonics Conference (IPC)

作者： Pavana Siddhartha Kollipara Linhan Lin Zhihan Chen Xiaolei Peng Yaoran Liu Yuebing Zheng The University of Texas Austin TX USA Materials Science and Engineering Program and Texas Materials Institute The University of Texas Austin TX USA State Key Laboratory of Precision Measurement Technology and Instruments Tsinghua University Beijing People’s Republic of China

Thermoelectric field around colloidal nanoparticles in laser-induced, spatially varying thermal gradients is theoretically derived. Experimental validation is also presented for diverse scenarios of laser-induced trap... 详细信息

ISBN: (数字)9781728158914

ISBN: (纸本)9781728158921

关键词： Laser theory Nanoparticles Nanobioscience Biomedical optical imaging Power lasers Temperature distribution Mathematical model

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Correction: High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

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Energy & Environmental science 2022年第4期15卷 1694-1694页

作者： Laisuo Su Harry Charalambous Zehao Cui Arumugam Manthiram Materials Science and Engineering Program & Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA Advanced Photon Source Argonne National Laboratory 9700 S. Cass Avenue Lemont IL 60439 USA

Correction for ‘High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology’ by Laisuo Su et al., Energy Environ. Sci., 2022, 15, 843–854, DOI: 10.1039/D1EE03103A.

Correction for ‘High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology’ by Laisuo Su et al., Energy Environ. Sci., 2022, 15, 843–854, DOI: 10.1039/D1EE03103A.

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The Role of Surfaces, Interfaces and Morphology on Silver Diffusion in Hard Coatings

SSRN

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SSRN 2023年

作者： Cavaleiro, Diogo Munnik, Frans Krause, Matthias Carbo, Enrique Ferreira, Paulo J. Cavaleiro, Albano Fernandes, Filipe University of Coimbra SEG-CEMMPRE - Centre for Mechanical Engineering Materials and Processes Department of Mechanical Engineering Rua Luís Reis Santos Coimbra3030-788 Portugal Helmholtz-Zentrum Dresden-Rossendorf Bautzner Landstrasse 400 Dresden01328 Germany INL – International Iberian Nanotechnology Laboratory Av. Mestre José Veiga s/n Braga4715-330 Portugal Mechanical Engineering Department IDMEC Instituto Superior Técnico University of Lisbon Av. Rovisco Pais Lisboa1049-001 Portugal Materials Science and Engineering Program The University of Texas at Austin AustinTX78712 United States IPN - LED&MAT - Instituto Pedro Nunes Laboratório de Ensaios Desgaste e Materiais Rua Pedro Nunes Coimbra3030-199 Portugal ISEP - School of Engineering Polytechnic of Porto Rua Dr. António Bernardino de Almeida 431 Porto4200-072 Portugal

One of the main approaches to increase the tool lifetime during dry machining of "hard-to-machine" aerospace alloys is self-lubrication by the incorporation of noble metals in hard matrixes with good mechanical and diffusion barrier properties. In this paper, the diffusion of an Ag-rich layer sandwiched between two layers of either TiN or TiSiN is studied by transmission electron microscopy and in situ Rutherford backscattering spectrometry. The layer stacks were subjected to annealing treatments at 600 ºC and 800 ºC for 2 hours. Three processes were found to control the diffusion of silver: the morphology of the "sandwich" layers, the formation of small voids in the involved interfaces and the sublimation of Ag in the surface at temperatures near the melting point. The study revealed that the dense TiSiN matrix allowed a significantly better control of Ag diffusion than the more open TiN matrix. © 2023, The Authors. All rights reserved.

关键词： High resolution transmission electron microscopy

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Thermally-induced phase transformations of CALF-20: insights into its phase stability and carbon capture properties

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Journal of materials Chemistry A 2025年

作者： Kang, Dong A. Suphavilai, Navaporn Mohamed, Amro M. O. Economou, Ioannis G. Shetty, Manish Kim, Jinsoo Jeong, Hae-Kwon Artie McFerrin Department of Chemical Engineering Texas A&M University 3122 TAMU College StationTX77843 3122 United States Department of Materials Science and Engineering Texas A&M University 3122 TAMU College StationTX77843 3122 United States Chemical Engineering Program Texas A&M University at Qatar PO Box 23874 Doha Qatar Kyung Hee University 1732 Deogyeong-daero Gyeonggi-do Yongin17104 Korea Republic of

Calgary Framework 20 (CALF-20) has garnered a great deal of attention as a promising adsorbent for CO2 capture applications due to its high CO2 uptake capacity and excellent stability in humid environments. Multiple studies have explored its adsorption properties and separation performance, while a few studies reveal the existence of several phases of CALF-20, including α-, β-, and τ-phases. α-Phase (i.e., referred as CALF-20) is known to transform into β- or τ-phase under humid or thermal conditions, respectively. Computational studies have shown that β-CALF-20 exhibits a higher heat of CO2 adsorption, making it more suitable for CO2 capture compared to α-CALF-20. However, β-CALF-20, transformed from α-CALF-20 under humid conditions, is known to be less stable, thus observed only upon moisture exposure. Here, we demonstrate that β-CALF-20 can be formed solely by thermal treatment of α-CALF-20 and this thermally-derived β-CALF-20 is significantly more stable and can be readily obtained by drying as-synthesized CALF-20 at temperatures above 100 °C. Computational analyses corroborate the experimental results, affirming that the α-to-β phase transformation can be achieved solely through thermal treatment, without the involvement of water, via a modification in the Zn coordination number from 5 to 4. More importantly, this study finds that it is challenging to determine gas adsorption properties of α-CALF-20, as degassing of α-CALF-20 at elevated temperatures under vacuum almost always leads to its transformation into β-CALF-20. The resultant β-phase demonstrates a CO2 uptake of 2.38 mmol g−1 at 0.1 bar and 30 °C, along with a CO2/N2 IAST selectivity of 222 for a 10 : 90 CO2/N2 mixture, which aligns with previous reports. Consequently, these findings imply that previously reported gas adsorption properties, including carbon (CO2) capture capacities, may have been measured on the β-phase of CALF-20, rather than the α-phase. © 2025 The Royal Society of Chemistry.

关键词： Metastable phases

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